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BY 4.0 license Open Access Published by De Gruyter October 22, 2021

Recent advances in waste-recycled nanomaterials for biomedical applications: Waste-to-wealth

  • Mohamed Abd Elkodous EMAIL logo , Hussein M. El-Husseiny EMAIL logo , Gharieb S. El-Sayyad EMAIL logo , Amr Hosny Hashem EMAIL logo , Ahmed S. Doghish EMAIL logo , Dounia Elfadil , Yasmine Radwan , Hayam M. El-Zeiny , Heba Bedair , Osama A. Ikhdair , Hisham Hashim , Ahmed M. Salama , Heba Alshater , Ahmed Ali Ahmed , Mahmoud Gamal Elsayed , Maria Nagy , Nouran Y. Ali , Maryam Elahmady , Ahmed M. Kamel , Mahmoud Abd Elkodous , Imene Maallem , Maria B. Sh. Kaml , Nayera Nasser , Ahmed AlaaEldin Nouh , Fatma M. Safwat , Mai M. Alshal , Salma K. Ahmed , Taha Nagib , Fatma M. El-sayed , Manal Almahdi , Yahia Adla , Noha T. ElNashar , Aya Misbah Hussien , Alaa S. Salih , Somaya Abdulbaset Mahmoud , Shireen Magdy , Diana I. Ahmed , Fayrouz Mohamed Saeed Hassan , Nermin A. Edward , Kirolos Said Milad , Shereen R. Halasa , Mohamed M. Arafa , Abdullah Hegazy , Go Kawamura , Wai Kian Tan and Atsunori Matsuda EMAIL logo
From the journal Nanotechnology Reviews

Abstract

Global overpopulation, industrial expansion, and urbanization have generated massive amounts of wastes. This is considered as a significant worldwide challenge that requires an urgent solution. Additionally, remarkable advances in the field of biomedicine have impacted the entire spectrum of healthcare and medicine. This has paved the way for further refining of the outcomes of biomedical strategies toward early detection and treatment of different diseases. Various nanomaterials (NMs) have been dedicated to different biomedical applications including drug delivery, vaccinations, imaging modalities, and biosensors. However, toxicity is still the main factor restricting their use. NMs recycled from different types of wastes present a pioneering approach to not only avoid hazardous effects on the environment, but to also implement circular economy practices, which are crucial to attain sustainable growth. Moreover, recycled NMs have been utilized as a safe, yet revolutionary alternative with outstanding potential for many biomedical applications. This review focuses on waste recycled NMs, their synthesis, properties, and their potential for multiple biomedical applications with special emphasis on their role in the early detection and control of multiple diseases. Their pivotal therapeutic actions as antimicrobial, anticancer, antioxidant nanodrugs, and vaccines will also be outlined. The ongoing advancements in the design of recycled NMs are expanding their diagnostic and therapeutic roles for diverse biomedical applications in the era of precision medicine.

Graphical abstract

Abbreviations

AC

activated carbon

Anti-EGFR

anti-epidermal growth factor receptor

BBB

blood–brain barrier

CT

computed tomography

CAs

contrast agents

CDs

carbon dots

CG

chitosan-doped graphene

CNCs

cellulose nanocrystals

CNFs

carbon nanofibers

CQDs

carbon quantum dots

CNMs

carbon nanomaterials

CNTs

carbon nanotubes

DCs

dendritic cells

Au NPs

gold nanoparticles

GO

graphene oxide

GQDs

graphene quantum dots

IO-CDs

iron oxide nanoparticle-doped carbon dots

IQDs

inorganic quantum dots

IO NPs

iron oxide nanoparticles

MOs

metal oxides

MNPs

magnetic nanoparticles

MPI

magnetic particle imaging

MRI

magnetic resonance imaging

MWCNTs

multi-walled carbon nanotubes

MIC

minimum inhibitory concentration

NMs

nanomaterials

NGO

nanographene oxide

PEG

polyethylene glycol

PEG-AuIONPs

PEG-coated iron-oxide–gold core–shell nanoparticles

QDs

quantum dots

ROS

reactive oxygen species

RNMs

recycled nanomaterials

rGO

reduced graphene oxide

SPIO NPs

superparamagnetic iron oxide nanoparticles

SWCNTs

single-walled carbon nanotubes

WCO

waste cooking oil

ZnO NPs

zinc oxide nanoparticles

1 Introduction

Since the emergence of the term nanotechnology, much effort has been dedicated to the investigation of the outstanding properties of nanomaterials (NMs) and their potential applications [1]. Materials having at least one dimension on the nanoscale (<100 nm) are identified as NMs [2]. NMs are quite fascinating and have wide applications in different fields such as biology, medicine, industry, energy, and so on [3,4,5,6,7].

Among all the possible applications of NMs, their biomedical applications are of particular interest and have led to the maturation of nanomedicine [8,9,10,11,12,13,14,15,16,17,18,19,20,21]. Various kinds of NMs have been prepared and their applicability has been extensively studied. NMs have shown the potential to overcome many severe drawbacks compared to other pharmacologically active agents and chemicals, including biological instability, lack of water solubility, and ineffectiveness in vivo [22]. Nowadays, NMs are used in many biomedical applications, such as drug delivery systems, treatment of diseases, early disease diagnosis, vaccines, biosensors, and bioimaging [23,24]. For the preparation of NMs, many methods have been developed, as shown in Figure 1.

Figure 1 
               Synthesis routes for NMs.
Figure 1

Synthesis routes for NMs.

However, there are concerns about the toxicity of NMs [25,26]. Thus, other more benign routes for the preparation of biocompatible NMs are important due to their interaction with the biological environment. Sustainability, referring to the production of NMs from everyday domestic and industrial wastes, can be a revolutionary solution and a route to achieve waste-to-wealth and zero-waste initiatives.

Many valuable NMs, such as carbon NMs (CNMs), gold nanoparticles (Au NPs), inorganic quantum dots (IQDs), and metal oxides (MOs) can be extracted from waste materials that include cooking oil, biomass, and industrial wastes. Interestingly, agricultural biomass wastes can be a valuable source for the green synthesis of NMs possessing many attractive properties such as lower toxicity, cost-effectiveness, tiny size, and higher stability [27]. These NMs have found many uses in biomedical applications [28,29,30,31,32,33,34].

More than 6 million tons of agricultural biomass is produced worldwide every year. Of this, 10% is produced in Europe (600,000 tons per year) [35]. Every year, huge amounts of waste cooking oils (WCOs) are produced worldwide, especially in developed countries [36]. In the USA, the daily estimation of WCO by the Energy Information Administration is 100 million gallons and the average per capita amount of WCO is reported to be nine pounds. The total WCO produced yearly in Canada is reaching approximately 135,000 tons [37]. In European Union countries, the amount of yearly WCO ranges from 750,000 to one million tons [38] and 200,000 tons are produced annually in the United Kingdom. Moreover, electronic waste (e-waste) has become a rapidly growing global concern. In European countries, 17 kg of e-waste per capita is produced yearly. In China and India, 1 kg of e-waste per capita is generated annually and includes Cu, Al, and iron metals [39]. According to the US Environmental Protection Agency, 4.6 million tons of e-waste entered US landfills in 2000 and that amount is rapidly increasing and expected to grow four-fold in coming years [40].

Within the past few years, a circular economy has become an important academic research domain. A significant increase in the number of articles addressing this topic has been published, as shown in Figure 2.

Figure 2 
               (a) Number of publications in the past ten years that address NMs (CNMs, IQDs, and MOs) recycled from biomass, cooking oil, and industrial wastes; (b) percentage according to waste type; and (c) percentage of each group of NMs.
Figure 2

(a) Number of publications in the past ten years that address NMs (CNMs, IQDs, and MOs) recycled from biomass, cooking oil, and industrial wastes; (b) percentage according to waste type; and (c) percentage of each group of NMs.

Further investigation on the progress of recycled NMs (RNMs) from wastes and their biomedical applications are of significant importance. In this study, various types of RNMs from three different sources (cooking oil, biomass, and industrial waste) are summarized. In addition, their synthesis, properties, and vital biomedical applications are presented. Our review offers a comprehensive, critical, and accessible overview of this innovative and sustainable trending topic.

2 NMs recycled from cooking oil, biomass, and industrial wastes for biomedical applications

2.1 Carbon-based NMs

2.1.1 Activated carbon (AC)

The AC available in the market is usually made from coal, lignite, peat, petroleum residue, and wood, which are known to be very expensive and exhaustible [41]. Chemical methods, such as chemical vapor deposition (CVD) and laser ablation, are the dominant fabrication methods for AC NPs, but these methods are toxic and highly expensive. Therefore, cooking oil waste, agricultural wastes, fruit peels, and industrial wastes, which cause many problems in the environment, have been used for CNM synthesis by green methods. Arie et al. [42] used WCO for CNM synthesis through nebulized spray pyrolysis while varying the processing temperature from 650 to 750°C.

Many researchers have used agricultural wastes as precursors for the production of AC for four primary reasons: renewable sources, cheap, readily available, and ecofriendly [43,44]. Agricultural wastes are widely used for the biosynthesis of AC [45,46]. Many studies have used olive stones for AC biosynthesis through ecofriendly methods [47,48], as well as walnut shells [49]. Yang et al. [50] used coconut shells via microwave heating for the production of AC. Another study biosynthesized AC from desiccated coconut waste [51] while AC was produced from Nicotiana tabacum stems using the carbonization process and KOH [52]. Gao et al. [53] synthesized AC from activated rice straw (RS), and AC particles were also produced from RS waste, which was applied in adsorption processes [54].

Fruit peels are considered one of the most important agricultural wastes. Fruit peels, such as banana peels [45], watermelon peels [55], bitter orange peels [56], cucumis melo peels [57], and durian peels [58], have been widely used for AC biosynthesis. Therefore, the utilization of the inedible parts of fruits (peels) may prove profitable for farmers in the near future since certain fruit peels are of great value as a source of bioactive compounds [59,60]. Potato peel from domestic and industrial waste was used for AC fabrication [61,62], and date seeds were used for the green biosynthesis of AC [63]. Likewise, Polyalthia longifolia seeds [64], African star apple seed husks, oil seeds, and whole seed [65] were validated. Additionally, stalks, such as arhar stalks [66] and grape stalks [67], were used to produce AC via the chemical activation method. Therefore, the use of these agricultural materials for the production of ACs makes them inexpensive and more efficient. Most agricultural wastes and fruit peel wastes used for AC biosynthesis are summarized in Table 1.

Table 1

Different types of recycled wastes used for the biosynthesis of NMs

NMs Wastes References
AC WCO [42]
Olive stone [47,48,49]
Walnut shell [49]
Coconut shell [230]
Nicotiana tabacum stem [52]
RS [53,54]
Banana peel [45]
Watermelon peel [55]
Orange peel [56]
Cucumis melo peel [57]
Durian peel [58]
Potato peel [106,288]
Date seed [288]
Polyalthia longifolia seed [64]
Star apple seed husk [65]
Arhar stalk [336]
Grape stalk [67]
CNFs Palm kernel shell [74]
Pine nut shell [75]
Walnut shell [78]
Sugarcane bagasse [73]
Palm fruit stalk [80]
Oil palm empty fruit and oil palm trunk [81]
Rice stems [82]
Banana peel [84]
Pine fruit wastes [85]
Liquid organic waste [86]
Shrimp shell [87]
Coal fly ash [88]
Waste tire [88]
CNTs Wheat straw [102,104]
Oat hull [102]
Rapeseed cake [102]
Hazelnut hull [102]
Sugarcane bagasse [103]
Potato peel [106]
Chickpea peel [107]
Banana peel [105]
G Waste cooking palm oil [108]
Chicken frying oil [32]
Oil palm fiber [127]
Peanut shell [110]
Tea tree plant extract [112]
Wheat straw [113]
Soybean shell [114]
Coconut shell [115]
Sugarcane bagasse [117,122,123]
Camphor leaf [116]
Alfalfa plant shoot [118]
Coir pith [119]
Rice husk [120]
Wild carrot root [121]
Bougainvillea glabra flower [124]
Mango peel [125]
Banana peel [126]
CQDs Frying oil waste [131]
Egg white and yolk [132]
Eggshell [133]
Sugarcane bagasse [122,142,143,144]
Peanut shell [145]
Coconut husk [146]
Tofu waste [147]
Beet [148]
Walnut shell [149]
Corn stalk shell [150]
Corncob residue [151]
Date kernel [152]
Mangosteen pulp [153]
Coconut shell [154]
Papaya waste pulp [337]
Rice residue [156]
Platanus waste [157]
Wheat straw [158,159]
Bamboo residue [159]
Banana pseudo-stem [160]
Onion peel [161]
Prawn shell [162]
Corn bran [163]
Tea stalk [164]
Coriander leaf [165]
Purslane leaf [166]
Azadirachta indica leaf [167]
Catharanthus roseus leaf [168]
Prosopis juliflora leaf [169]
Tea leaves [170]
Orange peel [174,175,176,177]
Watermelon peel [178]
Lemon peel [179]
Mango peel [181,182]
Pomegranate peel [179]
GQDs Cooking palm oil [186]
Rice husk [187,188,190,191,338]
Coconut husk [192]
Coffee grounds [190]
Sugarcane bagasse [193,194]
Bamboo timber waste [195]
Neem leaf [190,196,197]
Mango leaf [198,199]
Guava leaf [200]
Fenugreek leaf [197]
IO NPs Sugarcane bagasse [205]
Sorghum bran [206]
Eucalyptus leaf [207]
Carob leaf [208]
Ruellia tuberosa leaf [155]
Platanus orientalis leaf [209]
Green tea leaf [210]
Mango leaf [210]
Rose leaf [210]
Oregano leaf [210]
Curry leaf [210]
Oak leaf [211]
Pomegranate leaf [211]
Green tea leaf [211]
Grape leaf [212]
Garlic vine leaf [213]
Oolong tea leaf [214]
Salvia officinalis leaf [215]
Syzygium cumini seed [216]
Watermelon peel [217]
Orange peel [219,220]
Pomegranate peel [218]
Tangerine peel [221]
Aloe vera peel extract [222]
TiO2 NPs Calotropis gigantea (L.) Dryand leaf [231]
S. cumini leaf [232]
Psidium guajava leaf [233]
Orange peel [234,293]
Plum peel [228]
Peach peel [228]
Kiwi peel [228]
Tangerine peel [236]
Annona squamosa peel [227]
Watermelon peel [237]
ZnO NPs Rice husk [242]
Sugarcane bagasse [243]
Albizia lebbeck stem bark [244]
Potato peel [245]
Sheep and goat fecal matter [246,247]
Coriandrum sativum leaf [250]
Calotropis gigantea leaf [250]
Acalypha leaf [250]
Moringa oleifera [251]
Saffron leaf [252]
C. sativum leaf [253]
Aloe vera leaf [254]
Water hyacinth leaf [255]
Black nightshade leaf [256]
Santa maria leaf [257]
Banana peel [259,260,261,262]
Orange peel [263,264,265,266,267]
Pomegranate peel [268,269,270,271]
Rambutan peel [272]
Pineapple peel [273]
CuO NPs Cooking oil waste [281]
Sugarcane bagasse [282]
Walnut shell [284,285,286]
Zea mays L. dry husk [287]
Date stone [288]
Pomegranate leaf [289]
Andean sacha inchi leaf [290]
Brassica oleracea subsp. botrytis [291]
Eupatorium odoratum leaf [339]
Acanthospermum hispidum leaf [339]
Hylotelephium telephium flower [340]
Kalopanax pictus leaf [341]
Pterolobium hexapetalum leaf [342]
Juglans regia leaf [293]
Adhatoda vasica Nees leaf [294]
Blumea balsamifera leaf [295]
Ailanthus altissima leaf [296]
Orange peel [298,299]
Papaya peel [280]
Garcinia mangostana fruit pericarp [300]
Pomegranate peel [301,302]
Banana peel [303]
Lemon peel [299]
Au NPs Coconut oil [308]
Palm oil [309]
De-oiled jatropha waste [311]
Nepenthes khasiana leaf [312]
Crinum latifolium leaf [315]
Azadirachta indica leaf [316]
Coleus aromaticus leaf [317]
Elettaria cardamomum seed [318]
Abelmoschus esculentus seed [319]
Crocus sativus extract [316]
Cassava starch [313]
Nut shells [314]
Orange peel [324,332,333]
Pomegranate peel [325,326,327]
Banana peel [328,329]
Avocado peel [330]
Garcinia mangostana peel [331]
Watermelon peel [334]

2.1.2 Carbon nanofibers (CNFs)

CNFs belong to a new category of outstanding nanostructured materials due to their extraordinary mechanical and electrical properties [68]. In previous years, CNFs were manufactured using a variety of techniques such as laser ablation, arc discharge, sonochemical/hydrothermal methods, electrospinning, dry autoclaving, CVD, and the plasma-enhanced CVD process [69,70]. As these methods are toxic and expensive, wastes are now being used for CNF biosynthesis. WCO becomes an issue when solid waste laws prohibit liquids from being disposed of in landfills [71]. Utilizing WCO as a carbon precursor for the production of CNFs is a low-cost ecofriendly emerging technology. Indeed, mustard, turpentine, Eucalyptus, camphor, sunflower, palm, castor, and sesame oils have been proved to contain high carbon compositions [72]. The production of CNFs is fueled by the decomposition of hydrocarbon chains in oil [69].

Agricultural wastes, including plant shooting systems and wood, contain lignocellulosic materials such as lignin, cellulose, and hemicellulose [73]. In recent years, researchers have succeeded in the fabrication of CNFs from several different agricultural precursors. CNFs have been derived from palm kernel shell [74], and Zhang et al. [75] manufactured CNFs from pine nut shells by microwave pyrolysis. Furthermore, Wang et al. [76] reported that CNFs can be produced by the pyrolysis method using fir sawdust, bamboo, palm kernel shell, and pine nut shell. Likewise, loofah sponge was used to produce porous AC for use as a supercapacitor [77]. Porous CNFs produced from walnut shells were utilized as anodes in lithium-ion batteries [78]. In the same context, Chen et al. [73] produced highly effective CNFs from sugarcane bagasse and activated CNFs were also derived from hemp straw through carbonization and KOH [79]. In addition, CNFs can be fabricated from palm fruit stalks [80], oil palm trunk, and fruit bunches [81], which can be widely adopted for water purification. Furthermore, stems of rice plants were used as raw materials for CNF synthesis by the thermal decomposition method [82].

Industrial byproducts, that is, fruit peels, petrochemical wastes, or organic liquid wastes, could be used for CNF manufacturing. The fruit juice industry consumes fruits as juice and the peels are detached from the fleshy part of the fruit. These peels can be used as a carbon precursor for CNF production, thus reducing the environmental pollution resulting from the disposal of these wastes. Yadav and Sharma [83] prepared an extract from orange peels and utilized it as a precursor for CNF preparation by pyrolysis and chemical activation (using KOH). Likewise, banana peels were utilized for CNF biosynthesis [84]. Pine fruit wastes were also used as precursors for CNF synthesis by Shahba and Sabet [85]. Liquid organic wastes generated by petrochemical and chemical industries have been used to produce gas by electro-cracking; the gas acts as a carbon source for CNF manufacturing [86]. Moreover, shrimp shell wastes were used as a precursor of chitin nanofibers under acidic conditions utilizing a simple blending treatment [87], while coal fly ash and waste tires were utilized as precursors in CNF synthesis by pyrolysis [88]. Most of the agricultural and fruit peel wastes used for CNF biosynthesis are summarized in Table 1.

2.1.3 Carbon nanotubes (CNTs)

Nanocarbon material is a carbon-based material with a specified size and particle structure [42]. Numerous precursors of carbon, such as methane, acetylene, and benzene, have been used as carbon source material to synthesize CNTs [89,90,91]. In 1991, CNTs were discovered by Iijima as a cylindrical carbon nanostructure [92]. CNTs have been notable for many applications including energy storage electrodes in supercapacitors, polymers, gas storage materials, sensors, electronics, catalysts, and separation [34,93,94]. After the increase of environmental concerns and the growing demand for CNTs, many researchers have tried to increase CNT production while developing green technology [34]. CNT production is costly using traditional sources. So there is a need to find renewable resources for their production. Innovative research efforts that focus on the use of cost-effective and readily available renewable materials, like biomass, are required [95]. Therefore, the use of WCO is necessary, as it is generated from natural vegetable oils and animal fats that lose their nutritional value during the cooking process or deep processing [96]. The average amount of WCOs is remarkable worldwide and it may cause severe environmental, economic, and social problems [97]. The estimated worldwide annual production of waste vegetable oils is over 15 million tons, with around 1 million tons per year by the European Union [97,98,99]. WCO can be used as a starting material in the industrial-scale production of CNTs, which makes it both economical and environmentally beneficial [100].

Agricultural wastes have a high carbon content, with cellulose, hemicellulose, and lignin used extensively as carbon precursors [34]. Besides increasing its value, the use of cellulose-rich biomass (agricultural waste) would also help resolve environmental problems [101]. Therefore, renewable precursors should be widely used in future as they can be replenished fairly rapidly [95]. Hidalgo et al. [102] used wheat straw, oat hulls, rape seed cake, and hazelnut hulls as biomass waste for CNT production using a novel method of solvent self-ignition. Likewise, Mugadza et al. [103] produced nitrogen-doped multi-walled CNTs from sugarcane bagasse using the floating catalyst CVD method at 850°C. CNTs were synthesized from pretreated RS through the CVD of camphor [104]. Fruit peels were one of the agricultural wastes used for CNT synthesis. Mopoung [105] reported that banana peel mixed with mineral oil is the main precursor for the synthesis of CNTs. Another waste, potato peel, was used for the synthesis of CNTs for bio removal of heavy metals [106]. Moreover, chickpea peel waste was used for the synthesis of CNTs for bioimaging applications [107]. Most of the agricultural and fruit peel wastes used for CNT biosynthesis are summarized in Table 1.

2.1.4 Graphene (G)

G consists of pure carbon, wherein carbon atoms are arranged in a single layer to create a honeycomb pattern. It should be stressed that this layer of carbon is only one atom thick, although some authors consider up to ten layers of carbon to be G [108]. G is one of the most attractive CNMs due to its extraordinary electronic, optical, magnetic, thermal, and mechanical properties and wide applications [108,109]. There are many methods used in G synthesis, such as chemical synthesis, chemical exfoliation, mechanical exfoliation, and pyrolysis [109]. However, while these methods are very effective for G synthesis they are highly expensive and not ecofriendly. Therefore, there is a new direction in G synthesis by green methods using wastes, such as cooking oil, agricultural wastes, and industrial wastes. Robaiah et al. [108] verified waste cooking palm oil for G synthesis at different temperatures. In addition, Azam et al. [32] used palm-based waste chicken frying oil for G nanotablet synthesis.

Recently, scientists have been working on the large scale manufacture of G from biological sources like waste plant shells, plant aerial parts, plant seeds, biochar, eggshell, microorganisms, and even human hair [110]. Lignocellulosic agricultural wastes essentially consist of proteins, lignin, carbohydrates, cellulose, and hemicelluloses; their use for the production of adsorbents has piqued interest [110,111]. In this context, Jacob et al. [112] synthesized G from the tea tree plant (Melaleuca alternifolia) while Chen et al. [113] prepared value-added G from wheat chaff (Triticum sp.) by graphitization and hydrothermal methods, which were then applied in lithium-ion batteries. Furthermore, soybean shell (Glycine max) was used as a carbon precursor for G production by KOH followed by thermal treatment; it proved its efficiency in oxygen reduction reactions [114]. Likewise, Sun et al. [115] prepared G from the shell of coconut (Cocos nucifera) using ZnCl2 and FeCl3, and then used the resultant G as a supercapacitor. Additionally, ref. [110] used KOH for activation and then exfoliation to render G from peanut shells. Sugarcane bagasse and dried camphor leaves (Cinnamomum camphora) have also been validated in the biosynthesis of G [116,117]. G was produced from the aerial parts of alfalfa plants (Medicago sativa L.) with the oxidative action of HNO3 under a feasible process [118] and coir pith was used for G biosynthesis by a ball milling activation method [119]. Furthermore, G was synthesized using rice husk activated by KOH at 900°C for use in energy storage applications [120]. Kuila et al. [121] utilized wild carrot roots for the green biosynthesis of G oxide (GO) where the roots contain endophytic microorganisms responsible for the reduction process through an environmentally safe method. Baweja and Jeet [122] reported that sugarcane bagasse is an effective, economical, and suitable source for G biosynthesis. Likewise, Somanathan et al. [123] validated sugarcane bagasse for the biosynthesis of GO. Moreover, the flower extract of Bougainvillea glabra was used as a reducing agent for the biosynthesis of GO used in sensing applications [124].

Many fruits have been used for producing juice, syrup, nectar, sugar, or in the flavor industry. Consequently, large quantities of their waste products can be harmful to the environment. These byproducts are abundant in pectin, lipids, cellulose, proteins, hemicellulose, and enzymes, which can be exploited as raw material for G manufacturing [125]. Multi G layers were produced from mango peels on copper sheets using plasma [125]. Furthermore, highly effective antibacterial GO was produced from banana peel waste [126]. Tahir et al. [127] grew pure G on copper sheets by CVD using oil palm fiber and fruit trash. Ruan et al. [128] synthesized high-quality single-layered G from food wastes, for example, chocolate and cookie wastes, and solid wastes, for example, blades of grass, dog feces, and bulk polystyrene plastic, by CVD using hydrogen gas. Dung and the bones of cows, newspapers, and soot powders in diesel vehicle exhausts were used as precursors for G synthesis via the chemical exfoliation method [129]. Most of the agricultural and fruit peel wastes used for G biosynthesis are summarized in Table 1.

2.2 IQDs

2.2.1 Carbon quantum dots (CQDs)

CQDs are carbon NPs with a size less than 10 nm and have acted as surface passivation for inorganic materials. Moreover, they have good solubility, high stability, and are easily controllable by size and functional groups [130]. There is a need for clean materials in the synthesis of CQDs in the modern era of nanoscale materials. Previous studies have validated the use of agri-based wastes, such as frying oil waste [131], egg whites and yolks [132], and eggshells [133], for the synthesis of CQDs. Muthoni et al. [131] used frying oil waste as a precursor for the one-step synthesis of sulfur-doped carbon dots (CDs) with pH-sensitive photoluminescence. Egg yolk oil is known in traditional medicine in China and can be obtained by refining cooked egg yolks of Gallus domesticus Brisson [134]. Nowadays, focus has been on the preparation of CQDs from “green” materials with no chemicals included in the CQD synthesis and waste management utilized to create cheap and renewable materials with potential for commercial scale-up [135].

Agriculture wastes are considered a big threat to our environment as it is found within the soil as a byproduct from agriculture, industry, and domestic activities use [136]. However, most of these wastes are discarded, which cause environmental problems that threaten human health.

These wastes are known as renewable, naturally inviting, liberally accessible, and harmless carbon sources for carbon dot (C-dot) generation [137,138]. There are many types of these wastes such as sugar cane bagasse, coir, banana, and pineapple leaf, which cause pollution [139]. Sugarcane bagasse is one of the most abundant wastes, hence, efforts have been made to use it as a bio-fuel, in food products, and in carbon production [140,141]. Sugarcane bagasse was used for CQD biosynthesis via hydrothermal [142] and carbonization methods [143]. Sugarcane bagasse has also been used in CQD biosynthesis through a simple, efficient, economic, and sustainable approach [122,144]. Large amounts of peanut shells are dumped as waste every year. The quantity of waste peanut shells is huge and it is difficult to recycle [145]. Zhu et al. [145] used a novel method for synthesis of CQDs using peanut shells. Their generated CQDs were soluble in water. Chunduri et al. [146] reported that coconut husk can be used as a carbon source for the green synthesis of CQDs. Zhang et al. [147] synthesized two types of CQDs with tofu waste. Wang et al. [148] reported a strategy to prepare CQDs utilizing beet as the carbon source, as beets are rich in sucrose and other carbohydrates and are utilized to manufacture granulated sugar. Walnut shells were also used for the preparation of green photoluminescent CQDs, which are used in intracellular bioimaging [149]. Likewise, corn stalk shell [150], corncob residues [151], date kernel [152], mangosteen pulp [153], coconut shell [154], papaya waste pulp [155], rice residue [156], platanus waste [157], wheat straw [158,159], banana pseudo-stem [160], onion peels [161], prawn shells [162], corn bran [163], and tea stalks [164] were used for CQD biosynthesis by hydrothermal and carbonization methods. Additionally, plant leaf extracts, such as coriander [165], purslane [166], Azadirachta indica [167], Catharanthus roseus [168], Prosopis juliflora [169], and tea [170], were used for the green biosynthesis of CQDs. Fruit peel wastes have also been used for the green biosynthesis of CQDs. Banana peel is an agricultural solid waste that was used in the green hydrothermal synthesis of CQDs without the addition of any supplements [171,172,173]. Furthermore, orange peel [174,175,176,177], watermelon peel [178,179], lemon peel [180], mango peel [181,182], and pomegranate peel wastes [179] were used for the green and ecofriendly biosynthesis of CQDs. Most of the agricultural and fruit peel wastes used for CQDs biosynthesis are summarized in Table 1.

2.2.2 G quantum dots (GQDs)

GQDs are a new kind of quantum dot (QD) that have an intrinsic inert carbon property, which explains their chemical and physical stability [183]. Recently GQDs have received a lot of attention due to their unique properties, which include being environmentally friendly, non-toxic, biologically inert, biocompatible, and having high conductivity, broad surface area, low toxicity, and long lifetimes [184]. As a result of the high market cost of inorganic QDs, their industrial use has been limited. In addition, application development has been interrupted by the high toxicity of inorganic QDs. Therefore, the synthesis of GQDs from biowaste is considered a cost-effective alternative [185]. Cooking palm oil has been used for GQDs biosynthesis [186] and biomass, such as plant leaves, grass, coffee grounds, rice husks, and wood charcoal, stand out as a green, natural, cheap, sustainable, and renewable carbon source for the scalable production of GQDs [184]. Agricultural wastes, such as rice husk [187,188,189,190,191], coconut husk [192], coffee grounds [188,190], sugarcane bagasse [193,194], and bamboo timber waste [195], are widely used for the green biosynthesis of GQDs through ecofriendly methods. Moreover, plant leaf extracts, such as neem [190,196,197], mango [198,199], guava [200], fenugreek [197], and dried pine leaves have been used to synthesize GQDs [201]. Most of the agricultural and fruit peel wastes used for GQD biosynthesis are summarized in Table 1.

2.3 MO-based NMs

2.3.1 Iron oxide NPs (IO NPs)

IO NPs have shown many advantages for use in medicine and pharmaceutical applications. IO NPs are characterized by their low toxicity, high biocompatibility, and injectability; their magnetic and semiconductor properties have made them perfect candidates for drug delivery, magnetic resonance imaging, and cancer treatment and diagnosis [202]. Essential oils can be used to increase the stabilization of IO NPs as they have shown antimicrobial activity and can prevent pathogens from forming biofilms. These oils can be obtained from aromatic plants by steam distillation or mechanically from the pericarp [203].

Researchers continue efforts to develop facile, effective, and reliable green chemistry processes for the production of NMs. Recent studies have used agricultural wastes for IO NP synthesis [155,204]. Sugarcane bagasse was used to create magnetic IO NP for the removal of chromium ions from tannery effluent [205]. Njagi et al. [206] used waste sorghum bran to synthesize IO NPs using green technology. Leaf extracts, such as Eucalyptus [207] and carob [208], are widely used for IO NPs. Vasantharaj et al. [155] used the leaf extract of Ruellia tuberosa for IO NP biosynthesis through a green method that targeted photocatalytic degradation. Similarly, Devi et al. [209] synthesized ecofriendly IO NPs using the leaf extract of Platanus orientalis. IO NPs have been synthesized using green tea, mango, rose, oregano, and curry leaves [210]. Another study utilized oak, pomegranate, and green tea leaves and produced the richest extracts for green biosynthesis of IO NPs [211]. Similar studies also utilized grape leaf extract [212] and garlic vine leaf extract [213] for IO NPs through green and ecofriendly methods. Furthermore, Oolong tea and Salvia officinalis leaves were used in IO NP biosynthesis [214,215]. Venkateswarlu et al. [216] used the seed extract of Syzygium cumini for green biosynthesis of IO NPs.

Recent studies used fruit peel extract, such as watermelon rinds [217] and pomegranate peel [218], to create IO NPs through green and ecofriendly methods. Moreover, orange peel extract was used for IO NP biosynthesis [219,220] and IO NPs were synthesized in an ecofriendly manner from other peels such as tangerine [221] and Aloe vera extract [222]. Bishnoi et al. [223] validated Cynometra ramiflora fruit extract waste for the synthesis of magnetic IO NPs. Most of the agricultural and fruit peel wastes used for IO NP biosynthesis are summarized in Table 1.

2.3.2 TiO2 NPs

TiO2 NPs have been extensively studied because they have high quantum efficiency, application-appropriate electronic band structure, high specific surface area, chemical innerness, and stability [224]. TiO2 NPs are widely used in cosmetics and pharmaceuticals [225] and are also used as antibacterial agents [226]. Agricultural wastes, WCO, and fruit peel wastes are used in TiO2 NP biosynthesis through a green strategy [227,228,229].

Recently developed technologies have the potential to convert agricultural wastes into functional NPs. One important agricultural waste that may act as a promising biotemplate for the synthesis of TiO2 NPs is RS. It was demonstrated that mesoporous silica (MCM-41) obtained from rice husks enhanced the performance of TiO2-based photocatalyst for the degradation of trimethyl ammonium [230]. Another biomass waste of interest is the leaves of plants, which are incredibly useful for the production of MO NPs. Marimuthu et al. [231] reported that the leaf extract of Calotropis gigantea (L.) Dryand is promising for TiO2 NP fabrication. After 6 h, the extract contains primary amines that have an important role in the bioreduction of TiO2 to TiO2 NPs. Furthermore, Sethy et al. [232] used the leaves of S. cumini for producing TiO2 NPs through a non-toxic, simple, cost-effective, and ecofriendly fabrication method. Kalyanasundaram et al. synthesized TiO2 NPs from the aqueous leaf extract of Pithecellobium dulce and Lagenaria siceraria in 2018. Moreover, the aqueous leaf extract of Psidium guajava was used in TiO2 NP biosynthesis [233].

Orange peel extract from sweet orange (Citrus sinensis (L.)) was used in a green method for the synthesis of TiO2 NPs [234]. Additionally, Amanulla and Sundaram [235] synthesized TiO2 NPs from titanium tetra chloride using orange peel extract (C. sinensis), showing that the green biological synthesis methods used in preparing NPs exhibit better results compared to TiO2 NPs obtained chemically. Moreover, TiO2 NPs were synthesized by revalorization of agri-waste material such as peels of the rosaceous fruits Prunus domestica L. (plum), Prunus persica L. (peach), and Actinidia deliciosa (Kiwi), where the peel extract acts as reducing and capping agents [228]. Ajmal et al. [228] reported the ease, cost-effectiveness, economic viability, and useful biomedical property of the green chemistry approach for the biosynthesis of TiO2 NPs. Nanocrystals (NCs) produced with alternative synthesis methods transform the TiO2 precursor in TiO2 NCs using two volumetric ratios of tangerine peels (Citrus reticulata), an organic waste, as bio-mediator of chemical reactions [236]. The peel extract of Annona squamosa was utilized as a precursor for TiO2 NPs biosynthesis [227] and TiO2 NPs loaded onto AC prepared from watermelon peel waste were used for dye removal [237]. On the other hand, nanowaste management needs further study to determine their environmental impact, as it was reported that TiO2 NPs and ZnO NPs from sunscreen could have a role in the formation of free radicals in skin cells, which further damage to DNA and favor tumorigenesis and cancer development [238]. Most of the agricultural and fruit peel wastes used for TiO2 NPs biosynthesis are summarized in Table 1.

2.3.3 ZnO NPs

There is extensive research underway to commercialize NPs due to their remarkable features. There have also been huge efforts to synthesize different types of NPs from unconventional sources, like cooking oil. ZnO NPs are one of the MO NPs that can be used as an antimicrobial and antioxidant agent [239,240]. Agricultural biomass waste is considered one of the most common organic and nontoxic materials that could be used in several industrial domains. These agricultural biomasses mainly contain lignin, which is a byproduct from paper and pulp industries. Annually, tons of lignin are produced and more than 95% are dumped in rivers, which is a loss as it is an environmentally friendly product not being properly utilized [241]. The usage of lignin, which is cheap biomass, could serve two important purposes: reducing wastes and transforming them into valuable materials, instead of dumping in rivers and causing major pollution. This transformation could be done through ZnO NP production from safe sources.

Agricultural wastes, such as rice husk [242], sugarcane bagasse [243], and Albizia lebbeck stem bark [244], are widely used for the green biosynthesis of ZnO NPs. Moreover, potato peels have been used for the biosynthesis of ZnO NPs, which were in turn used to target photocatalytic activity against methylene blue [245]. Other wastes can also be used in the biosynthesis process, such as sheep and goat fecal matter [246,247]. Chikkanna et al. [248] used sheep and goat fecal matter as a reducing agent for the production of ZnO NPs.

Ali et al. [249] explained the importance of utilizing green sources, such as leaves, roots, or shoot powders and flowers, in a form of solvent-based extract as stabilizing or capping agents to synthesize pure ZnO NPs. Leaf extracts from sources such as Coriandrum sativum plant leaves, C. gigantea leaves, and Acalypha leaves [250] have also been used for the biosynthesis of ZnO NPs. Surendra et al. [251] used Moringa oleifera for the biosynthesis of ZnO NPs and applied them for their antimicrobial activity. Rahaiee et al. [252] used the leaf extract of saffron as a reducing and stabilizing agent for ZnO NP production through a facile green approach. Furthermore, the leaf extract of C. sativum was also used for ZnO NP production [253]. Other leaf extracts, such as Aloe vera [254], water hyacinth [255], black nightshade [256], and Santa maria [257] have been used in the ecofriendly biosynthesis of ZnO NPs.

Fruit peel wastes are an ecofriendly and economic source for ZnO NP production. Peels of tomato, orange, grapefruit, and lemon were used for green biosynthesis of ZnO NPs [258]. More recent studies used banana peel extract for ZnO NP synthesis. The synthesized ZnO NPs were used in different applications due to their antimicrobial, antioxidant, and anticancer actions, and in photocatalytic degradation [259,260,261,262]. Furthermore, orange peel extract was used for the green synthesis of ZnO NPs that were applied in antibacterial activity, strawberry preservation, and photocatalytic degradation [263,264,265,266,267]. Other fruit peel wastes, such as pomegranate [268,269,270,271], rambutan [272], and pineapple peels [273], have also been used in the synthesis of ZnO NPs. Most of the agricultural and fruit peel wastes used for ZnO NP biosynthesis are summarized in Table 1.

2.3.4 CuO NPs

Copper is considered an important trace element in humans, animals, and plants [274]. CuO NPs have received much attention in recent years due to their wide application in many fields [275]. General applications of CuO NPs concern antimicrobial, antioxidant, and anticancer materials, gas sensors, conducting materials, magneto resistant materials, remediation, and biological removal of dyes and heavy metals [276,277,278]. In the last two decades, wastes, such as frying oil, agricultural, and industrial wastes, have been widely used for the synthesis of CuO NPs [279,280]. CuO NPs were synthesized in situ within ionic liquid-in-vegetable oil micro-emulsions [279]. Sarno et al. [281] prepared Cu NPs directly from WCO through a green strategy.

There have been various challenges in the production of biomass-assisted MO NPs, like CuO NPs, from agricultural wastes. Kumar et al. [282] reported that the biosynthesis of MO NPs using agricultural wastes is essential as these wastes are renewable sources, cheap, safe, and environmentally friendly. Agricultural wastes, specifically the lignocellulosic wastes such as rice husk, straws, and walnut shells, are very well known for their availability and low cost. Sugarcane bagasse [282,283], walnut shells [284,285,286], Zea mays L. dry husk [287], and date stones [288] have been used for green biosynthesis of CuO NPs.

Leaf extracts, such as those from pomegranate [289], Andean sacha inchi [290], Brassica oleracea subsp. botrytis (L.) [291], Eupatorium odoratum, Acanthospermum hispidum, Hylotelephium telephium, Kalopanax pictus, and Pterolobium hexapetalum [292], Juglans regia [293], Adhatoda vasica Nees [294], Blumea balsamifera [295], Ailanthus altissima [296], and Drypetes sepiaria [297], have also been used to create CuO NPs. Furthermore, fruit peels, such as orange peel [298,299], papaya extract (Carica papaya L.) peel waste [280], Garcinia mangostana fruit pericarp [300], pomegranate peel extract [301,302], banana peel [303], and lemon peel [299], were used for the green and ecofriendly biosynthesis of CuO NPs. Most of the agricultural and fruit peel wastes used for CuO NP biosynthesis are summarized in Table 1.

2.4 Au NPs

There are various techniques for Au NP synthesis, such as chemical reduction, microwave, ultraviolet radiation, photochemical, and sonochemical methods [304,305]. While these methods are effective for the biosynthesis of Au NPs, they are toxic and expensive. Therefore, green methods using WCO, biomass, and agricultural wastes are an optimistic approach toward NP synthesis in a clean, simple, safe, and environment friendly manner [306,307]. Au NPs are a bio-based product that can be synthesized using WCO, which is a cheap and renewable stock for biomedical products when efficiently collected and recycled. Otherwise, if WCO is illegally disposed of many environmental problems may occur [71]. Coconut oil has been used as a reducing and stabilizing agent for the synthesis of Au NPs, which were spherical with varied particle sizes [308]. Likewise, Sadrolhosseini et al. [309] reported the synthesis of Au NPs dispersed in palm oil (as a stabilizing agent) at different temperatures using the laser ablation technique. Palm oil is characterized by long hydrocarbon chains, which prevent NP agglomeration, and polar ester bonds, which can cap the NPs.

Agricultural wastes used for Au NP biosynthesis depend on upcoming methods that reduce the target biomass by converting Au(iii) to Au(0), forming Au NPs. Armendariz et al. [310] utilized wheat and oat (Avena sativa) biomass and successfully confirmed Au NPs with different morphologies, including face-centered cubic (FCC) tetrahedral, decahedral, hexagonal, etc. Moreover, fungal biomass can be used as it too has reducing capability. Kanchi et al. [311] used de-oiled jatropha waste for Au NP synthesis. Recent research projects synthesized Au NPs from the leaf extract of Nepenthes khasiana [312], liquefied mash of cassava starch [313], macadamia nut shell waste [314], and Crinum latifolium leaf [315]. Additionally, Crocus sativus liquid extract, A. indica leaves [316], and the leaf extract of Coleus aromaticus [317] were used for Au NP biosynthesis through green and ecofriendly methods. Seeds of an herbaceous plant called Elettaria cardamomum (of the ginger family whose seeds contain many phytochemicals) are capable of reducing gold ions and stabilizing formed NPs [318]. Also, the seed aqueous extract of Abelmoschus esculentus was utilized for the biosynthesis of Au NPs and their fungal activity was evaluated [319].

Fruit peel wastes are a promising source for the synthesis of metallic NPs, such as Au NPs, where their extracts act as a reducing agent in the synthesis [320,321]. The recycling of these biomass wastes makes it an environment-friendly method due to efficient management and usage [322]. Different fruit wastes, such as grape, jatropha, mango peel, banana peel, and watermelon rind wastes, were successfully used for Au NP synthesis [323]. Castro et al. [324] reported the use of orange peel for the synthesis of Au NPs wherein the initial pH was adjusted to control their size, shape, and structure. Furthermore, pomegranate peel waste is widely used for the conversion of HAuCl₄ to Au NPs for biomedical applications [325,326,327]. In the same context, banana peel waste was used for Au NP biosynthesis [328,329] while Adebayo et al. [330] used an aqueous extract of avocado (Persea americana) fruit peel to synthesize spherical and FCC Au NPs. In addition, G. mangostana fruit, sweet orange (C. sinensis), and Citrus maxima peel extracts have all been approved for Au NP synthesis, confirming that fruit wastes are a promising resource for Au NP stability and synthesis [331,332,333]. Chums-ard et al. [334] synthesized Au NPs using the red and green parts of watermelon waste. The red part extract formed spherical and hexagonal plates of Au NPs while the green part waste formed triangular NPs. Likewise, watermelon peel waste has been confirmed useful for the biosynthesis process [335]. Most of the agricultural and fruit peel wastes used for Au NP biosynthesis are summarized in Table 1.

3 Synthesis and properties of RNMs

3.1 Carbon-based NMs

3.1.1 AC

The use of fruits and vegetable peels as an activator for carbon has prevailed for the purification of aqueous environments. In 2009, orange peels were used for waste water purification and the orange peels were then used with lemon peels to produce AC [343]. Many other agricultural wastes and biomass seeds have been used to produce AC, such as potato peels, which were used in the treatment of pharmaceutical effluents [344,345] and to absorb heavy metals from aqueous media [61].

Torres et al. extracted soybean peroxidase (SP), a residue with large carbon and moderate ash content [345]. This residue was applied as a carbonaceous precursor to provide AC with a high surface area (1,603 m2 g−1), as shown in Figure 3. The waste originating from SP was washed with distilled water, dried at 60°C for 24 h, then treated with zinc chloride, and pyrolyzed in a tubular oven under an N2 flow at 550°C for 3 h. The produced AC was used as support for SP immobilization for different biomedical and pharmaceutical applications.

Figure 3 
                     Removal of soybean hulls to produce AC and scanning electron microscopy (SEM) images of precursor (soybean hulls) for AC (a) after activation with ZnCl2 and (b) after immobilization at different magnifications (c) and (d). Copyright © 2017, Royal Society Publishing Group [345].
Figure 3

Removal of soybean hulls to produce AC and scanning electron microscopy (SEM) images of precursor (soybean hulls) for AC (a) after activation with ZnCl2 and (b) after immobilization at different magnifications (c) and (d). Copyright © 2017, Royal Society Publishing Group [345].

With industrial and technological development and the emergence of the plastic waste crisis, many researchers have used polyethylene terephthalate (PET) to produce AC. PET was used for the first time in 1999 by Marzec et al., who investigated the effect of the adsorption capacity of carbon [346]. The preparation of AC from a precursor rich in carbon content has received attention. The AC can be produced in two ways: physical and chemical activation [347]. Two steps are required in the physical activation method: first is the carbonization of the precursor material, which takes place at a temperature that ranges from 400 to 800°C, and the second is activation, which takes place at a very high temperature, beginning from 800°C and reaching 1,000°C in the presence of the oxidizing agent (CO2 or air). A complete list of the methods are noted in Tables 2 and 3 [347].

Table 2

Different physical methods for AC production from biomass with corresponding properties

Material Activating agent Temperature (°C) Surface area (m2 g−1)
Coconut shell [347] CO2
Corncob [347,348] CO2 800 919–986
Rice husk [347] CO2 700 and 750
Rice husk [349] Hydrothermal carbonization 243
Almond tree pruning (non-catalytic gasification) [347,350] Air 190 116–469
Almond tree pruning (catalytic gasification) [347] Air 190–260 959
Olive tree wood [347,351] Air 400 413
Corn Stover [351] Microwave pyrolysis 1671.4 
Table 3

Different physical methods for AC production from industrial wastes with corresponding properties

Material Carbonization Carbonization temperature (°C) Activating agent Activating temperature (°C) Surface area (m2 g−1)
PET [352] Under N2 800 N2 and CO2 975 790
Polyvinyl chloride(PVC) [353] Air 900 Steam 900 1,000–2,000
Refuse paper and plastic fuel [353] Wet N2 (20% steam) 500
Sawdust [354] Under N2 CO2 700, 720, 740, and 760 302–405
Sawdust [355] N2 isotherms CO2 flow and by pyrolysis 200–900
Paper mill waste [356] 300 Steam 850 135.49

Additionally, chemical activation can be done in one step and at a low temperature. Therefore, many researchers prefer to use this method to save time and money. The chemical agent represents the oxidant and dehydrating agent added to the precursor and mixed at a temperature less than 800°C, as noted in Tables 4 and 5 [347]. No result was found regarding the use of WCOs to prepare AC. The use of AC for filtration of cooking oil meant for use as pet food [357] and as a homogenous catalyst to prepare biodiesel from WCO [358] has been reported.

Table 4

Different chemical methods for AC production from biomass with corresponding properties

Material Activating agent Temperature (°C) Surface area (m2 g−1)
Potato peel [143] H3PO4, KOH, and ZnCl2 400, 600, and/or 800
Rice husk [351] KOH 750 2,696
Rice husk [351] H3PO4 500 1,741
Rice husk [351] ZnCl2 500 2,434
Peanut shell [351] KOH 706.1
Coconut shell [351] ZnCl2 900 332.4
Coconut shell [351] KOH 900 682.0
Banana peel [351] KOH 800 217.3
Soybean [351] KOH 2690.3
Wheat straw [351] KOH 1,066
Pomelo peel [351] KOH 1,533
Pomelo peel[351] H3PO4 1,272
Citrus peel [351] KOH 1,167
Olive stone [351] KOH 587
Table 5

Different chemical methods for AC production from industrial wastes with corresponding properties

Material Carbonization Carbonization temperature (°C) Activating agent Activating temperature (°C) Surface area
PET [346] N2 for AC-a 402 m2 g−1 for AC-a
N2 + H2O for AC-b 359 m2 g−1 for AC-b
CO2 for AC-c 50 FeCl3 500 123 m2 g−1 for AC-c
PET [353] N2 600 KOH in a nitrogen stream 850 2,831 and 2,666 m2 g−1
PVC [353] Air 300 KOH in the presence of nitrogen 750
Refuse paper and plastic fuel [353] K2CO3 1,330 m2 g−1
Sawdust [359] KOH 500, 1876.16 m2 g−1

3.1.2 CNFs

CNFs have been in history for over a century. In an 1889 patent, carbon filaments were reported to be made from carbon-containing gases using a metal crusher as a catalyst [360]. Ghosh et al. was considered the first to describe the interaction between methane, metal surfaces, and graphical carbon at relatively low temperatures [361]. In 2019, catalytic decomposition of biogas over a Ni: Co/Al2O3 catalyst was generated in a rotator bed reactor by fishbone-type CNFs.

Agricultural waste (nutshell and wheat straw) has been used to manufacture AC. The applied method was respectful of the environment and the total cost of production was reduced. Fe and Ca in biomass derived ACs have a total content of less than 3%. The main steps involved to form CNFs on AC are the decrease in iron particles with H2, the dissociated ethylene chemical adsorption of some faces in iron particle antipersonnel, a dispersal of carbon species created during decomposition by the catalyst particle, and solid carbon precipitation on other metal faces to form a fibrous structure. Suriani et al. [362] validated chicken fat waste for CNF production. The ecofriendly consequences of their contribution are shown in Figure 4. The waste commodity of the poultry industry has significantly interfered with the field. The main fatty acids recently reported in chicken fat are oleic, palmitic, and linoleic acids. This initial study resulted in the synthesis of CNFs using an easy and viable CVD process with chicken waste fat and skin [363]. A dry rendering process was used to extract chicken oil from the chicken fat and skin. The fat and skin were heated to 200°C to isolate the liquid oil from the solids. The oil was filtered and then blended directly with ferrocene at 5.33 wt%. The oil-purified mixture was thoroughly stirred for 30 min and 6 mL was cross sprayed in a vaporization furnace at 470°C, followed by 60 min of synthesis performed at 750°C. Brief descriptions of the synthesized CNFs and their significant characteristics were provided. The CNFs were described as urchin-like (urchin being a marine creature). The clusters were composed of a multi-needle-like nucleus, with a diameter of 146 nm, and radially developed from the heart, as presented in Figure 4 [364].

Figure 4 
                     (Bottom) SEM images of CNFs synthesized using waste chicken fat. Copyright © 2015, Elsevier Publishing Group [362].
Figure 4

(Bottom) SEM images of CNFs synthesized using waste chicken fat. Copyright © 2015, Elsevier Publishing Group [362].

Sami et al. [86], showed that CNFs developed with different morphology and graphitization degrees through decomposition of the electrical cracking gas on Fe2O3. Compared to conventional physical methods, such as laser ablation and CVD, the benefits of this process are CNFs with high performance, high selectiveness, and low cost. The use of electric cracking gas to synthesize CNFs is promising [86]. It enables organic liquid waste from the chemical industry to be used while carbon and hydrogen are obtained at moderate temperatures. The synthesis of CNFs was done using an integrated reactor based on a fluid laboratory design. The electrical cracking gas was removed from the electrical gas storage using a valve, regulated by a valve, and operated by a water U-tube manometer at atmospheric pressure. Physical, morphological, chemical, and environmental features of produced nanofibers were studied by scanning electron microscopy (SEM). Many advanced properties were exhibited wherein the catalytic decomposition was shown to be the main pathway for CNF growth [365].

3.1.3 CNTs

Suriani et al. [100] produced CNTs from refined domestic cooking palm oil that was used to fry three loads of fish. The synthesis process was carried out in a floating-catalyst thermal CVD reactor. Alves et al. [366] synthesized CNTs from sugarcane bagasse supplied from the ethanol industry. In that study, pyrolysis was used in which the materials were decomposed by a thermal treatment in the absence of oxygen. Qu et al. [367] synthesized CNTs by heating leaves of poplar to 450°C in air and Suriani et al. [368] succeeded in the production of vertically aligned CNTs by catalytic thermal CVD using waste chicken fat and skin collected from a wet market and then converted into carbon precursor through a rendering process.

Bernd et al. [371] produced CNTs through pyrolysis of wood sawdust in a tubular reactor and Lotfy et al. [369] applied a novel pyrolysis system to prepare CNTs from RS, which is considered an undesirable biomass in Egypt. Singh et al. [370] succeeded in the synthesis of CNTs from polyvinyl alcohol (PVA) using fly ash, red mud, and rock samples via an alkali treatment followed by the fabrication of thin films and pyrolysis of composite films. Finally, Bernd et al. [371] synthesized carbon nanostructures by the pyrolysis of wood sawdust in a tubular reactor, as shown in Figure 5. Table 6 summarizes the different methods used for the production of CNTs and their corresponding properties.

Figure 5 
                     Schematic of the preparation of CNTs with corresponding particle size determination using high resolution transmission electron microscopy (HRTEM) imaging [371].
Figure 5

Schematic of the preparation of CNTs with corresponding particle size determination using high resolution transmission electron microscopy (HRTEM) imaging [371].

Table 6

Different synthesis methods and corresponding properties of CNTs

Method of preparation Carbon source Type and shape of CNTs Catalyst and temperature Diameter Surface area Notes References
WCO
Catalytic cracking WCO model compound Few multi-walled CNTs and some CNTs with an open-top structure Catalyst: Ni-Co/SBA-15 catalysts 50–100 nm [96]
Temperature: 750°C
Waste biomass
Pyrolysis Wood sawdust Single and double-walled CNTs Catalyst: Ferrocene or Fe/Mo/MgO 25 nm Wood sawdust was mixed with reducing agents (commercial zinc), calcite (bed material), and catalyst and arranged in the column reactor, as shown in Figure 5 [371]
Temperature: 750°C for 3 h
Pyrolysis Hydrocarbons of: Type of CNTs depends on the type of RS precursor Catalyst: Fe-Ni oxides supported on Al2O3 The diameter of CNTs differ according to the type of RS precursor The surface area of CNTs from raw RS is 188 m2 g−1 Hydrothermal treatment was carried out to produce hydrocarbons as an intermediate carbon source [369]
Raw RS Multi-walled CNTs (from raw RS and RS-neutral) Raw RS (from 15 to 40 nm)
RS-neutral pulp Needle-shaped CNTs (from RS-AP and RS-SP) Temperature: 750°C for 120 min RS-NP (from 14.7 to 47.9 nm)
RS-alkaline pulp (AP) RS-AP (from 2.5 to 6.8 nm)
RS-sulfite pulp (SP) RS-SP (from 4 to 8 nm)
Hydrothermal + temperature calcination approach Recyclable plant Typha orientalis Nitrogen-doped CNTs Catalyst: – CNTs: 150 nm 281.3 m2 g−1 [372]
Temperature: 180°C for 12 h, washed, freeze dried, and annealed at 800°C for 1 h in NH3 atmosphere Pore diameter: 4 nm
Industrial wastes
Pyrolysis Fly ash, red mud, and rock sample Different types of CNTs Catalyst: – 20–30 nm CNTs from: fly ash (42.3 m2 g−1), red mud (38.8 m2 g−1), and rock sample (19.7 m2 g−1) [373]
Temperature: 500°C for 20 min

3.1.4 G

Renewable biomass resources are essential for G precursors such as glucose, rice husk, hemp, and disposable paper cups. Recently, glucose was used as a preparatory material for G with the aid of FeCl3. The obtained G had effective electrical conductivity [374]. Researchers also synthesized “patched graphene,” G produced using glucose with the aid of dicyandiamide (DCDA). The author of this study claimed the resulting G to be highly crystalline and clean. Luyi et al. succeeded in the production of biocompatible G from rice husk [375377]. The obtained G could be used for bioimaging and bioprobing [188]. Fibrous hemp waste was successfully converted to G by Wang et al. [378] while Zhao obtained high quality and high yield G using disposable paper cups as a precursor [379]. Industrial wastes, such as plastic, can be used as precursors for G production. A group of researchers developed an approach to produce G from various wastes and food using CVD. This new approach is sensible, however, its yield is a matter of concern [374]. The production of G from WCO is a very interesting topic to many researchers. Recently, a group of researchers developed a method to produce G from waste cooking palm oil due to the presence of palmitic acid, CH3(CH2)14COOH, which is the source of carbon. Consequently, this method indicates the possibility of using waste cooking palm oil to obtain G at a low cost and without consumption of fossil fuels [380].

Graphite and organic materials are fundamental sources for the preparation of G. The approach of each method to prepare G, CVD on metallic films [381], liquid exfoliation of graphite crystal [382], mechanical cleavage [383], growth on silicon carbide [384], and chemical reduction of GO [385], has been illustrated by Ren and Cheng [386].

Glucose extracted from vegetable waste (as biomass) was first used to produce G in the presence of FeCl3 [387]. Initially, the glucose and FeCl3 were dissolved in water at 80°C to form carbonized glucose and FeCl2 (H2O2). The production of G was obtained at 700°C. DCDA was added to glucose in the presence of nitrogen to form graphite carbon nitride (g-C3N4) [388]. At a temperature higher than 750°C, G sheets were obtained, as shown in Figure 6.

Figure 6 
                     Proposed synthesis method for free-standing G. Bottom: repetition motifs of an ideal g-C3N4 plane (middle) and of G (right); C is indicated by black or gray, N is indicated by blue. Copyright © 2012, Wiley Publishing Group [387].
Figure 6

Proposed synthesis method for free-standing G. Bottom: repetition motifs of an ideal g-C3N4 plane (middle) and of G (right); C is indicated by black or gray, N is indicated by blue. Copyright © 2012, Wiley Publishing Group [387].

Biomass material, like hemp, can be converted to G by the hydrothermal method [378]. In this technique, fibrous hemp is heated around 180°C for an entire day. Then, KOH is added to produce porous G. Disposable paper cups can be used as a precursor for G production. In this approach, iron has been used as a catalyst to form Fe3C layers by heating the activated paper cup at high temperatures [379]. Industrial waste, such as plastic, is also a good source of carbon for G production. CVD is the most common approach to produce G from industrial waste [128]. Finally, cooking palm oil is an organic molecule that has been used as a precursor for G production via double thermal CVD using nickel as the deposition surface with variable temperature (850–1,100°C in 50°C increments) [389].

3.2 IQDs

3.2.1 CQDs

Biomass has a high carbon and oxygen content and is a non-toxic and widely available feedstock, making it a fascinating CQD source. Currently, several agricultural, forestry, and food waste types, such as rice husk, wheat straw, sugar cane bagasse, soya, onion, peanut cotton shell, potato, durian, and fruit/vegetable peel (orange, banana, pineapple, onion, seaweed, watermelon peel, etc.), have been utilized to manufacture low-cost CQDs [390,391]. Several precursors have been used for the preparation of CQDs, including banana peel waste, while using easy and green hydrothermal methods without passivates or additives [392].

By using red cabbage (RC) and a one-step hydrothermal method, Sharma et al. [393] evaluated a green method for the creation of CQDs. Yang et al. [394] studied expired fruits as carbon sources for the preparation of CQDs and Luo et al. [395] prepared CQDs using loofah sponge-based AC fiber as the raw material. Zhang et al. [396] used black soya beans (BS) as a cheap source of carbon for the green synthesis of BS-CQDs. Such high-value CNMs, such as the CQDs, can be synthesized using other abundant waste, such as low-cost petroleum coke byproducts and humic acid. Tajik et al. [397] also described the graphitic framework of petroleum coke with benzene or aromatic fields, which permits a chemical oxidation process for the synthesis of CQDs.

Compounds such as chitosan, citric acid, urea, and ascorbic acid, as well as a variety of foods, plants, waxes, and wastes, such as peels (mango, orange, banana, pineapple, onion, seaweed, etc.), egg yolk oil, meat, grains, nuts, or vegetable byproducts, have been used in the synthesis of CQDs. These compounds are low cost starting material for the creation of carbon materials [398]. Due to their green chemistry, hydrothermal and solvothermal methods are ecofriendly, mass-producible, cost effective, clear, and applicable for the synthesis of CQDs using various organic sources [393]. Başoğlu et al. [399] studied a simple CQD green synthesis method that used rusty chickpea as the single-stage carbon source, with no chemical additives. In another example, expired passion fruit shell (EPFS) and pulp were separated physically and the EPFS was cleaned using pure water. Then, the EPFS was placed into a furnace at 120°C for 28 h. After drying, the EPFS was crushed into a fine powder and placed into a 60-mesh sieve. Next, 2 g of EPFS powder with 40 mL of ultra-pure water was added to a polytetrafluoroethylene lined reactor and heated for 3 h at 175°C. Then, the received brown solution was filtered by a polyether sulfone membrane and centrifuged for 20 min at 15,000 rpm. After centrifugation, the product was dialyzed using a 2,000 days dialysis bag for two days. After the dialysis, the solution was freeze-dried to achieve the desired solid CQDs. The obtained CQDs were uniformly dispersed and spherical, with a size below 5 nm, indicating good dispersion (Figure 7).

Figure 7 
                     Proposed synthesis technique for powder CQDs by the hydrothermal method and corresponding transmission electron microscopy (TEM) images at different magnifications. Copyright © 2021, Springer Publishing Group [399].
Figure 7

Proposed synthesis technique for powder CQDs by the hydrothermal method and corresponding transmission electron microscopy (TEM) images at different magnifications. Copyright © 2021, Springer Publishing Group [399].

3.2.2 GQDs

High-quality GQDs with a yield of ∼15 wt% were prepared from rice husk biomass by Wang et al. [188]. Also, GQDs were produced utilizing a low-cost, green, and renewable biomass resource via microwave treatment by Abbas et al. [400]. Recently, scientists have targeted the transference of 2D G into 0D GQDs and studied the impact of edge effects and quantum confinement on the properties of the new material [401]. GQDs are synthesized from molecules with aromatic structures (biomass and cooking oils) where the formation of GQD moieties can undergo a step-by-step chemical reaction by molecular precursors. These approaches allow for excellent control of the properties of the final product [401,402].

The synthesis of GQDs from a low cost, green, and renewable biomass resource, rich in carbon, was achieved using microwave treatment of carbon biochar through the pyrolysis of biomass waste. Increasing the reaction time or microwave power resulted in an increase in the product yield (∼84% yield was achieved) [400]. Wang et al. [188] synthesized high-quality GDQs from rice husk biomass and it was found to be a useful source that produced a yield of ∼15 wt%. HRTEM, atomic force microscopy, and Raman spectroscopy were used to determine the size, structure, and morphology of the rice husk, as shown in Figure 8.

Figure 8 
                     Proposed synthesis for powder GQDs by the hydrolysis method and corresponding TEM imaging. Copyright © 2016, ACS Publishing Group [188].
Figure 8

Proposed synthesis for powder GQDs by the hydrolysis method and corresponding TEM imaging. Copyright © 2016, ACS Publishing Group [188].

3.3 MO-based NMs

3.3.1 Iron oxide

Bishnoi et al. [223] used the extract of C. ramiflora, an inedible fruit waste, for the synthesis of magnetic IO NPs. C. ramiflora belongs to the leguminosae family. It is largely found in Africa, as shown in Figure 9, and is used for biomedical and environmental applications.

Figure 9 
                     Biosynthesis of IO NPs using Cynometra ramiflora leaf extract for biomedical and environmental applications.
Figure 9

Biosynthesis of IO NPs using Cynometra ramiflora leaf extract for biomedical and environmental applications.

Additionally, IO NPs have been synthesized using tangerine peel extract and used as an adsorbent for cadmium ion removal from contaminated solutions. Ehrampoush et al. [221] prepared IO NPs by the co-precipitation method in the presence of tangerine peel extract, which prevented accumulation and reduced the diameter of the synthesized IO NPs. Sundaram et al. [403] isolated the Bacillus subtillis bacterial strain from rhizosphere soil to produce IO NPs through the fermentation process. Khan et al. [404] described the synthesis of superparamagnetic IO NPs in bio char from the condensed tannin extract of Acacia mearnsii. They utilized a single-step process compliant with the principles of green chemistry. By the warm deterioration of iron oleate within sight of sodium oleate (from biomass waste), Xie et al. [405] integrated IO NPs with different shapes. By tuning the molar proportion of sodium/iron oleate or the response temperature, plates, tetrahedrons, octahedrons, curves, multi-branches, or self-gathered designs could be achieved (Figure 10).

Figure 10 
                     Example morphologies of 0D IO NPs synthesized from iron oleate and sodium oleate (biomass wastes): (a) nanospheres, (b) plates, (c) tetrahedrons, (d) cubes, (e) truncated octahedrons, (f) octahedrons, (g) concaves, (h) octapods, and (i) multi branches [405].
Figure 10

Example morphologies of 0D IO NPs synthesized from iron oleate and sodium oleate (biomass wastes): (a) nanospheres, (b) plates, (c) tetrahedrons, (d) cubes, (e) truncated octahedrons, (f) octahedrons, (g) concaves, (h) octapods, and (i) multi branches [405].

Another study [155] synthesized IO NPs utilizing R. tuberosa leaf fluid concentrate and their ultraviolet-visible spectroscopy investigation showed obvious tops at 405 nm. Dynamic light dissipation determined the normal size of IO NPs to be around 52.78 nm and differential scanning colorimetry demonstrated the strength of IO NPs until reaching the high temperature of 165.52°C.

Promptly after adding iron sulfate to the leaf extract, IO NPs were shaped and in this manner, the technique is straightforward and quick [406]. In this investigation, a basic, fast, and eco-accommodating green technique was used to create magnetite IO NPs utilizing the fluid concentrates of two food-handling wastes, in particular the velvety hairs of corn (Zea mays L.) and external leaves of Chinese cabbage (Brassica rapa L. subsp. pekinensis). The bubbled arrangements of satiny hairs (MH) and external leaves of Chinese cabbage (CCP) were utilized to blend IO NPs under photograph uncovered conditions [407]. Another study revealed that C. maxima peel extract yielded IO NPs with a diameter of 10–100 nm and high stability [408].

3.3.2 TiO2

TiO2 NPs have been prepared from biomass, cooking oils, and industrial waste through chemical, physical, and biological approaches. There are also different chemical methods to create TiO2 NPs, such as sol–gel, solvo-thermal, hydrothermal, and co-precipitation methods [409]. Table 7 summarizes the different chemical methods used to fabricate TiO2 NPs from biomass and their corresponding properties.

Table 7

Different chemical methods for the synthesis of TiO2 NPs and their corresponding properties

Material Method Initial temperature (°C) Final temperature (°C) Pressure (bar) Surface area (m2 g−1) Size (nm)
RS [229] Sol–gel 80 500 97 13.0 ± 3.3
Eggshell [410] Solvothermal 454 227 78.73

On the other hand, physical methods, such as electrophoretic, thermal plasma, spray pyrolysis, and microwave-assisted techniques, have been applied for TiO2 NP synthesis from different biomass wastes [409]. Biological synthesis methods (also called green synthesis methods), use plants and fruit extracts, in addition to their waste materials and microorganisms (via fermentation methods), for the synthesis of NMs, to reduce the use of costly, toxic chemicals. Thus, they are considered as cost-effective and ecofriendly methods [409]. Table 8 summarizes the different biological methods used for the synthesis of TiO2 NPs from microorganisms and fruit peel extracts with their corresponding properties.

Table 8

Different synthetic biological methods, and corresponding properties of TiO2 NPs

Material Initial temperature (°C) Final temperature (°C) Size (nm)
Orange peel extract [235] 100 500 21.61 and 17.30
Plum peel extract [228] 70–80 400–500 47.1 and 63.21
Peach peel extract [228] 70–80 400–500 200 
Kiwi peel extract [228] 70–80 400–500 54.17 and 85.13 
Sugar-apple [411] 23
Aeromonas hydrophila [411] 40.50
Bacillus amyloliquefaciens [411] 22.1–97.2
Bacillus mycoides [411] 40–60
Bacillus subtilis [411] 30–40
Lactobacillus sp. [411] 24.63
Planomicrobium sp [411] 100
Aspergillus niger [411] 73.58

3.3.3 ZnO

Ramimoghdam et al. [412] suggested a method for recycling waste oil for the synthesis of ZnO NPs. The group used palm olein, the liquid fraction of palm oil, as a bio-template to synthesize NPs with different morphologies. Bio-templating is the use of a biological structure that serves as a template, guiding the assembly of inorganic materials into NPs of the desired morphology.

Industrial waste first supplied a pure zinc source in 2011 when Deep et al. [413] dismantled spent Zn–MnO2 batteries, separated their metal components, and used the purified zinc for NP synthesis. In a later study, Deep et al. (2016) [414] also used spent Zn–MnO2 batteries to propose a simpler, more efficient synthesis method: a one-pot solvothermal process. This method resulted in the isolation of highly pure ZnO NPs at a recovery percentage ≥95%. Farzana et al. [415] similarly synthesized ZnO NPs from Zn–C spent batteries.

The use of microbial biomass (nanofactories), acting as reducing and capping agents through the fermentation process, was first investigated by Jayaseelan et al. [424] for the preparation of ZnO NPs by adding ZnO to a suspension of Aeromonas hydrophila bacteria. More recent studies have reported the use of C-phycocyanin pigment from cyanobacteria in the synthesis of phycocyanin–ZnO nanorods [417]⁠ with the use of zinc-tolerant Lactobacillus plantarum [425].

Agricultural waste and inedible plant leaves and peels are also being used as bio-reductants for green ZnO NP synthesis, mainly due to their polyphenolic content. Different wastes have been used for the biosynthesis of TiO2 NPs, such as rambutan peel [272], M. oleifera peel [251], and agricultural waste [426], which contains bioreductant and secondary metabolites such as terpenoids, alkaloids, and flavonoids. In 2020, ZnO NPs were synthesized using orange peel [427], non-edible cauliflower leaves [291], garlic skin extract [428], and banana peel [429]. In 2021, Rambabu et al. [423] used date pulp waste to synthesize ZnO NPs. Table 9 includes all the methods applied for ZnO NP synthesis from industrial waste, biomass, and cooking oils.

Table 9

Different waste materials and synthesis methods used to create ZnO NPs with different sizes and morphologies

Source of waste material Type of waste material Zinc source Type of synthesis Name of synthesis method Reaction temp. (°C) Calcination temp. (°C) Size (nm) Morphology Ref.
Industrial waste Spent Zn–MnO2 batteries Zinc extracted from waste electrode material Chemical Solvothermal synthesis 250 NA 5 Spherical [414]
Industrial waste Spent Zn–C batteries Zinc from waste electrode material Chemical Thermal nanosizing 900 NA 50 Spherical [416]
WCO Palm oil Zinc acetate Chemical Hydrothermal method using palm olein as a bio-template 120 NA Micro- and nano-sized particles, depending on the volume of palm olein added and reaction time Different morphologies, depending on the volume of palm olein added and reaction time [412]
Microbial biomass Phycocyanin extract from Cyanobacterium Limnothrix sp. K005 Zinc acetate Biological (fermentation) NA 30 NA 33–35 Nanorods [417]
Microbial biomass Serratia nematodiphila Zinc sulfate Biological (fermentation) NA NA NA 15–30 Spherical [418]
Plant biomass Moringa oleifera peel extract Zinc acetate Biological + physical Microwave-assisted synthesis Microwave power of 300 W 400 and 600 40–45 Spherical [419]
Plant biomass Sheep and goat fecal matter (agri waste) Zinc sulfate Biological NA Room temperature 350–400 24.4–28.5 Spongy and flower shaped [248]
Plant biomass Orange peel extract Zinc nitrate Biological NA 60 400 Different sizes depending on reaction temperature and pH Different morphologies depending on reaction temperature and pH [263]
Plant biomass Cauliflower leaf extract Zinc nitrate Biological NA Sonication at 30 NA 100 Spherical [419]
Plant biomass Pectin from durian rind Zinc acetate Biological NA Room temp. NA 280–456 Spherical [420]
Plant biomass Pectin from banana peel Zinc acetate Biological + chemical Co-precipitation Room temp. NA 20–40 Thin flakes, nanocones, flower-shaped, and cubic-shaped [421]
Plant biomass Banana peel extract Zinc acetate Biological NA NA NA 20–90 Spherical, triangular [422]
Plant biomass Garlic skin extract Zinc chloride Biological NA NA NA 7.77 Rod shaped, hexagonal [428]
Plant biomass Date pulp waste Zinc nitrate Biological NA Room temp. 400 30 Spherical [423]

3.3.4 CuO

The green biosynthesis of CuO NPs from different waste materials, such as cooking oil, biomass (including plants and microorganisms), and industrial wastes, is common, as shown in Figure 11. Javed et al. used waste palm oil as a base solvent for the synthesis of ecofriendly, highly stable, and bio-renewable CuO NPs [430]. The synthesis of CuO NPs using bio-waste plant peels, lignocellulosic biomass-rich materials, and seed extract, such as citrus peel (orange, lemon, and tangerine) [430,431], banana peel (Musa acuminate) [303,432], pomegranate peel (Punica granatum) [302,433,434], pomegranate seeds [435], papaya peel (C. papaya) [280], date stone [434], Zea mays husk [435437], onion peel (Allium cepa) [438], fava bean seed peel [439], cauliflower (B. oleracea), potato (Solanum tuberosum) and pea (Pisum sativum) peels [440], and Colocasia esculenta leaf waste has been reported (Table 10) [441]. Recycling a variety of industrial wastes is a low-cost and safe method for CuO NP production. CuO NPs have been recovered from Cu-rich industrial waste, such as e-waste that includes SIM cards [442] and printed circuit boards (PCBs) [443446], batteries, including LIBs and NiMH batteries [447], waste sludge [448,449], and wastewater (Table 11) [450].

Figure 11 
                     An illustration of the green synthesis of CuO NPs from waste materials by different physical, chemical, and biological methods.
Figure 11

An illustration of the green synthesis of CuO NPs from waste materials by different physical, chemical, and biological methods.

Table 10

Green synthesis methods for producing CuO NPs from waste materials and their properties

Method Waste material Cu precursor Size Shape Yield Process Advantages Ref.
Industrial wastes
Physical Waste PCBs (WPCBs) PCBs of old telephones and PCs 5–40 nm Spherical 90% Electro-kinetic (EK) method Simple, ecofriendly, and cost effective [444]
Chemical Waste SIM cards Waste mobile SIM cards 2–50 nm Cauliflower like 95.3% Wet chemical method Simple and ecofriendly [442]
WPCBs WPCBs Different sizes Irregular sheet 98% Mechanochemical method Simple and ecofriendly [445]
WPCBs Old computer WPCBs 15–16 nm Spherical Over 90% Chemical reduction “hydrometallurgical approach” Cost effective/ecofriendly, high pure particles. [451]
WPCBs Copper-containing waste etchants and CuCl2 2–50 nm Spherical >99.90% Microemulsion Simple, economical, and safe, with low energy consumption, high production yield with high purity (>99.0%) [443]
WPCBs WPCBs and CuSO4 Spherical 96.9% Chemical reduction Simple, ecofriendly, cost effective, high production yield [452]
Wastewater Wastewater from electroplating industry and CuSO4 20–80 nm Crystalline 99.98–99.99% Precipitation method Economic and safe process, with high production yield [450]
Wastewater sludge Industrial wastewater 200–400 nm Feather like 90% Hydrometallurgical method by acid leaching Simple, cost effective, and high production yieldwith high purity 98.26% [449]
Waste oil
Biological and chemical Palm oil Copper nitrate 25 nm Spherical Precipitation method Simple, cost effective, and economic process [430]
Plant wastes
Biological and chemical Lemon pulp CuCl2 20–40 nm Irregular 103 mg/g Hydrothermal method Simple, rapid, ecofriendly, and cost effective with high yields [453]
Waste bamboo leaf Copper acetate 70–80 nm Hierarchical Hydrothermal method Simple, rapid, ecofriendly, cost effective, high production yield [454]
Onion peel Copper chloride 11.7–45.5 nm Berry-like Microwave-assisted Simple, rapid, ecofriendly, cost effective [438]
Biological and physical Fava bean seed peel Copper sulfate 29.82 nm Spherical Gamma radiation Simple, rapid, ecofriendly, cost effective [439]
Biological method Banana pulp waste Copper acetate 1–4 µm Octahedral Banana pulp waste extract as a reductant Simple, green, ecofriendly [455]
Banana peel Copper sulfate 50–60 nm Spherical Banana peel extract as a reductant Simple, green, ecofriendly [432]
Pomegranate peel and date stone Copper sulfate 6–20 nm Crystalline Pomegranate peel and date stone extract as a reductant Simple, green, ecofriendly [434]
Pomegranate peel Copper chloride 5–25 nm Rod and spherical Pomegranate peel extract as a reductant Simple, rapid, safe, with low energy consumption [433]
Pomegranate seeds Copper nitrate Broccoli Pomegranate seeds extract as a reductant Simple, green, ecofriendly [435]
Citrus peel Copper nitrate 22.4–94.8 nm Spherical Citrus peel extract as a reductant Simple, green, ecofriendly [431]
Papaya peel Copper nitrate 85–140 nm Crystalline Papaya peel extract as a reductant Simple, rapid, cost effective [280]
Zea mays husk Copper acetate 20–70 nm Spherical Waste maize extract as a reductant Simple, green, eco- and economically friendly [437]
Brown algae Macrocystis pyrifera Copper sulfate 2–50 nm Spherical Brown algae extract as a reductant Simple, ecofriendly [456]
Table 11:

Various waste materials for CuO NP synthesis and their corresponding properties

Waste material Cu precursor Size (nm) Shape Ref.
Plant wastes
  Citrus peel (orange, lemon, and tangerine) Copper nitrate 22.4–94.8 and Spherical and [430]
8–8.9 irregular [431]
  Banana peel Copper acetate 7.33 Spherical [457]
60 [303]
  Pomegranate peel Copper acetate and 10–100 Spherical [302]
Copper sulfate 6 Crystalline [434]
  Pomegranate seeds Copper nitrate Broccoli [435]
  Papaya peel Copper nitrate 85–140 Crystalline [280]
  Date stone Copper sulfate 20 Crystalline [434]
  Zea mays husk Copper acetate 36–73 Spherical [436]
20–70 Spherical [437]
  Onion peel Copper chloride Berry like [438]
  Cauliflower peels, potato peels, and pea peels Copper chloride <100 Irregular [440]
  Colocasia esculenta leaf Copper nitrate <100 [441]
Industrial wastes
  e-waste Waste mobile SIM cards 2–50 Cauliflower like and spherical [442]
  SIM cards Waste telephones, PCBs 11, 25, and 40 [444]
  PCBs PCBs and chloride (CuCl2) 20–50 [443]
  Wastewater Copper sulfate 20–80 Crystalline [450]

3.4 Au NPs

The synthesis of NPs using chemical methods is usually associated with the formation of toxic byproducts. Therefore, the use of biosurfactants/biological materials (biomasses like microbes and plants) for the synthesis and stabilization of Au NPs is gaining importance since a decade [458]. The microbial route for the synthesis of Au NPs is a very exciting process, as several factors including microbial cultivation methods on organic and/or inorganic wastes and extraction techniques can be optimized for the fast synthesis of monodispersed NPs by the fermentation process. Many biological systems such as those of fungi [459] and algae [460] have been studied for the biosynthesis of Au NPs.

A newer Au NP synthesis technique includes materials such as oat and wheat biomasses, which have been shown to reduce aqueous gold ions to gold zero-valent forming Au NPs [310]. Recently, a method was developed for the preparation of Au NPs that involves application of an alternating current voltage to metal electrodes in an electrolyte solution containing a water-soluble polymer dispersant and a reducing agent [461]. A method for the extraction of gold from waste electrical and electronic equipment as NPs stabilized with phospholipids was suggested using 1,2-dioleoylsn-glycero-3-phosphocholine [461].

WCO contains long hydrocarbon chains and polar ester bonds that make it a good choice for stabilizing Au NPs. In this preparation method, Au NPs are synthesized in WCO using the laser ablation technique at different temperatures. A gold plate (high impurity 99.99%) was immersed in 10 mL of pure palm oil, which was extracted from WCO. A laser beam of 532 nm wavelength, with a period and energy of 10 ns and 1,200 MJ, respectively, was used to ablate the gold plate at different temperatures for 5–60 min with a 30–60 Hz repetition rate. The solution temperature was raised using a hot plate. Au NPs formed during the laser ablation with an ablation time of 25 min. This experiment was conducted at different temperatures (40, 64, 75, 83, and 92°C). The solution was stirred during the ablation and the solution container was moved horizontally to obtain a fresh surface area for the Au NPs to guarantee that the Au NPs were dispersed equally in the WCO [309].

Velmurugan et al. [462] synthesized Au NPs from ginger waste, which includes the aqueous extract of waste ginger. Ginger waste acts as both a reducing and stabilizing agent. For a typical synthesis, 5 mL of the extract is added to 3 mL of freshly prepared 1 mM solution of HAuCl4. The mixture was allowed to boil by rapid microwave heating. The appearance of the red color in the reaction mixture indicated the formation of Au NPs. The colored solution of Au NPs was then centrifuged, and the Au NPs were redisposed to remove any unreacted ions and molecules from the product. The produced Au NPs were highly stable and spherical, with diameters of 15.5 nm.

Liu et al. [463] synthesized Au NPs from banana peel by the hydrothermal process. After mixing with HAuCl₄ as the precursor, the banana peel was heated with water and acetone at 98°C. No extra chemical protectant or reductant was added. Finally, Au NPs with four leaf clover (dendrite) morphology were obtained, which were named Au dendrites, as indicated in Figure 12.

Figure 12 
                  Simplified diagram of the synthesis process of Au dendrites and the different shapes with their corresponding colors. Copyright © 2020, Dove press Publishing Group [463].
Figure 12

Simplified diagram of the synthesis process of Au dendrites and the different shapes with their corresponding colors. Copyright © 2020, Dove press Publishing Group [463].

4 Biomedical applications of RNMs: Role of RNMs in the early detection of diseases

4.1 Fluorescence imaging

Biological components are too small to be observed by traditional microscopy, which lacks the accuracy and high-resolution localization to image the biological processes inside these components. A fluorescent dye fixes this problem by providing several optimal approaches to track cells and evaluate their functionality. Fluorescence imaging is a common tool used to visualize precious molecular mechanisms [464,465], gene and protein expressions [466468], and interactions between cellular components, providing a deeper understanding of the biological process.

The advantages of fluorescence imaging over other imaging techniques are high selectivity of the desired area, high-resolution power, identification of microelements inside the cellular component, and production of high-contrast images [469]. Fluorescent NPs have promising qualifications for fitting the small size of the cellular components while providing more abilities compared to other fluorescent techniques, such as a low cytotoxicity level, better selectivity, smooth entrance, the ability to target a large number of cells at the same time, low chemical structure changes, and high-throughput screening [470,471].

Long-period cellular tracking in vivo provides valuable information regarding the biological process and biomedical therapeutics. Several biological imaging modalities have been developed for those applications, including magnetic resonance imaging (MRI), magnetic particle imaging (MPI), and fluorescence imaging. Merging nanotechnology with these methods has improved the safety of cellular tracking in vivo and has overcome some challenges of traditional imaging methods. Compared to conventional fluorescent methods, fluorescent NPs support the unique advantages of photofading resistance, higher brightness, and better size control [472]. Cellular tracking fluorescent NPs are inorganic QDs [473,474], nanodiamonds [475], fluorescent latex/silica nanobeads [476], and organic NPs [477].

The early detection of diseases is currently a critical point of focus in clinical practices. One of the most prominent examples is the early detection of cancer. It was reported that patients who were diagnosed early with gastrointestinal cancer had a higher survival rate than those who did not benefit from early detection (92.3% versus 33.3%) [478]. One of the key players in the early detection of diseases is biomedical imaging, which includes MRI, positron emission tomography, ultrasound, X-ray radiography, single-photon emission computed tomography, computed tomography (CT), and fluorescence imaging [479]. However, structural imaging modalities, such as CT, ultrasound, and MRI, are not useful in the detection of some tumors due to their detection limitations (0.5 cm) and spatial resolution. Imaging modalities can be combined to improve the efficiency of tumor detection [480]. Contrast agents (CAs) are used to provide accurate functional and anatomical information. Medical imaging CAs usually used are small molecules that have low undesirable toxicity, non-specific distribution, and fast metabolism. However, nanoimaging CAs are currently being studied extensively due to their outstanding properties compared to traditional CAs. Nanoimaging CAs exhibit a high surface-area-to-volume ratio, leading to enhanced surface functionalization and lower toxicity profiles [481]. Additionally, nanoimaging CAs exhibit a longer plasma circulation time and better biodistribution and bioavailability, thus enhancing the tumor-to-background contrast signal. Furthermore, the manipulation of NP properties allows optimized loading of imaging compounds [482,483].

4.2 Role of NPs in fluorescence imaging

Fluorescence imaging technology is currently widely used for disease diagnosis as it provides the highest spatial resolution compared to other imaging technologies [484]. However, fluorescence imaging in clinical settings is hindered by some limitations, including non-specific tissue auto-fluorescence, and limited penetration depth. Also, photobleaching effects and limited fluorescence in the target site decrease the sensitivity of the technology for disease detection [483,485487].

NMs play a key role in the enhancement of fluorescence imaging to overcome limitations. Near infrared (NIR) fluorescence quenching could be avoided by using modified NPs [488]. NPs could also reduce photobleaching effects by converting low-energy photons into high-energy photons [489]. In addition, NPs allow the loading of more dye molecules, thus providing higher signals [490]. NPs could also be targeted to tumors or target sites through passive or active targeting, allowing accumulation in desired sites and increasing the fluorescent dye concentrations and thus the signal. Hence, fluorescent NPs are being extensively developed and investigated for biomedical applications [483]. For example, NP fluorescence imaging is currently used in several biomedical applications, such as enzyme activity evaluation, gene detection, cell tracking, protein analysis, real-time monitoring of therapeutic effects, and early detection of diseases [490493]. For cancer diagnoses, fluorescent NPs play a crucial role as they provide high-resolution images at the cellular level. Examples of promising fluorescent NPs include QDs, organic dye-doped NPs, upconversion NPs, and Au NPs [494]. The different examples of NPs used in fluorescence imaging for early detection of different diseases are provided in Table 12.

Table 12

Selected examples of NPs recycled from different wastes and employed in fluorescence imaging for early detection of different diseases

Authors NPs Waste source Disease diagnosed/cells imaged Ref.
Zhou et al. (2012) CQDs Waste watermelon peel HeLa cells [178]
Hu et al. (2014) CQDs doped with sulfur Waste frying oil HeLa cells [513]
Park et al. (2014) CQDs Food waste HepG2 cells/Liver Carcinoma [514]
Xue et al. (2105) CQDs Lychee seed HepG2 cells [515]
Xue et al. (2016) CQDs Peanut shell waste Multicolor imaging of HepG2 live cells [516]
Yao et al. (2017) Gd@CQDs Crab shell waste HeLa and HepG2 cells [517]
Bankoti et al. (2017) CQDs co-doped with nitrogen, sulfur, and phosphorous Culinary onion peel waste MG63 and HFFs cells [518]
Manaf et al. (2017) CQDs Sago bark industrial biowaste N2a and melanoma A-375 cells [519]
Cheng et al. (2017) CQDs Walnut shell biowaste MC3T3 cells [520]
Cheng et al. (2019) N/S-CQDs Cellulose-based biowaste from willow catkin HeLa cells [505]
Anthony et al. (2020) Recycled CQDs Rice waste A549 cells [551]
Ding et al. (2018) GQDs Lignin biowaste RAW 264.7 cells, monocytes/macrophage-like cells [552]
Zhang et al. (2019) N-GQDs Marigold plant Detecting of Fe3+ ions as a target for bioimaging inside the living cells [553]

4.3 CQDs for early disease detection via fluorescence imaging

Fluorescence imaging has gained increasing attention recently due to its high sensitivity, selectivity, and high-throughput ability. Developing optimum fluorescent probes has always been a challenge. QDs are inorganic semiconductor NCs that possess exceptional photophysical characteristics. Based on their quantum properties, QDs can emit a wide and broad spectrum of different fluorescent wavelengths that give them preference for use in biomedical applications, particularly in the tracking of circulating tumor cells and early diagnosis of abnormal tumor masses [495497]. Briefly, QDs are made from a metallic-semiconductor core that includes elements of both II–VI (e.g., ZnSe, CdTe, CdS, and CDSe) and III–V (e.g., InAs and InP) groups of the periodic table, which are coated with a shell of biomolecules, like polysaccharides, peptides, or proteins, to prevent the leakage of toxic heavy metals and to provide good stability for the NP in a biological environment.

Although QDs have shown highly promising results among traditional fluorescent probes, it has been found that QDs exhibit some toxic effects, which limit the applications of heavy metal QDs. Alternatively, using safe, cost-effective, and ecofriendly materials that have been recycled from biological wastes has become a trend since they are readily available and less toxic. For example, CQDs produced from recycled biomass waste have been applied in fluorescent imaging.

CQDs are small nanostructures with carbon as the core element. Currently, this type of QD has received much interest due to its unique properties, including its size (below 10 nm), chemical stability, wide range of fluorescence emission, high availability, easy synthesis, and water solubility. The fluorescence of CQD emission ranges in the NIR spectrum and, in addition, CQDs have low physiological toxicity compared to semiconductor QDs, making them a superior choice for biomedical applications. The biomedical applications of CQDs are in vitro and in vivo bioimaging, drug delivery [498,499], tumor mass detection [500], and cancer therapy [501503].

One of the main properties of CQDs is their fluorescence, which promotes their application in fluorescence imaging. Narrow emission spectrum, wide excitation spectrum, high fluorescence stability, and resilient resistance to photobleaching are all outstanding fluorescence properties of CQDs [137]. However, these excellent CQD properties are affected by the CQD source, such as CQDs biomass wastes. A study by Zhang et al. reported that the organic solvent used for CQDs affected the fluorescence emission peak position and fluorescence emission intensities of CQDs synthesized from polystyrene foam waste [504]. Another study by Cheng et al. stated that CQDs co-doped with nitrogen or sulfur and prepared from cellulose-based biowaste showed low cytotoxicity, good biocompatibility, and high fluorescence quantum yield and, thus, could be used in intracellular imaging applications [137,505].

The potential applications of CQDs in bioimaging have got much attention, particularly in cellular imaging. This application was first applied in 2006 to stain human colorectal adenocarcinoma cells (Caco-2 cell line) in vitro [398]. Additionally, several attempts have been made on different cell lines in vitro, such as HeLa [506,507], HepG2 [507], and A549 cells [508], for internal imaging. Also, bioimaging in vivo has been reported since researchers have managed to track murine alveolar macrophage in vivo [509], human neural stem cells [510], cardiac and pancreatic progenitors [511], as well as imaging ClO-ions inside nude mice [512].

Zhou et al. used waste watermelon peel for large-scale synthesis of CQDs. The produced CQDs exhibited high stability in a high salinity solution and a wide range of pH values with exceptional water solubility. The system was effectively used in fluorescence imaging of HeLa cells. Thus, the produced CQDs could be used as optical imaging probes in biomedical applications [178]. Moreover, Hu et al. demonstrated the synthesis of pH sensitive fluorescent CQDs doped with sulfur from waste frying oil for imaging and sensing of pH changes in HeLa living cells. The obtained CQDs exhibited high photostability, good fluorescence quantum yield, and low cytotoxicity, making them biolabeling probe candidates for imaging living cells [513].

Park et al. used ultrasonic treatment for the large-scale production of CQDs from food waste. The produced CQDs exhibited high photostability, good fluorescence, low toxicity, and high water solubility. The CQDs were used for the fluorescence imaging of human hepatocellular liver carcinoma (HepG2) cells and the nuclei of the cells produced a strong, red-colored fluorescence, indicating the ability of the CQDs to penetrate the cells while maintaining their properties intracellularly [137,514].

Xue et al. produced CQDs from lychee seeds by one-step pyrolysis. The CQDs exhibited low cytotoxicity, excellent biocompatibility, and could be used as an ecofriendly material for in vitro and in vivo bioimaging applications in cell biology and other sensing applications. Moreover, these CQDs were used for the fluorescence imaging of HepG2 live cells [515].

Another study conducted by Xue et al. used peanut shell waste to produce CQDs via the pyrolysis technique. The produced CQDs exhibited excellent photostability, high stability for a wide range of pH values, low photobleaching, outstanding biocompatibility, and low cytotoxicity. The CQDs were used as a fluorescent probe for multicolor imaging of HepG2 live cells. Bright blue, green, and red fluorescence were observed in the cytoplasm upon excitation at 405, 488, and 514 nm, respectively [516].

Yao et al. demonstrated the synthesis of magneto fluorescent CQDs through a one-pot microwave-assisted hydrothermal method using the transition metal ions Gd3+, Mn2+, and Eu3+ and crab shell waste. The formed Gd@CQDs were conjugated to folic acid (FA) and doxorubicin (DOX). The conjugated Gd@CQDs allowed specific targeting and fluorescence imaging of HeLa and HepG2 cells and displayed high cytotoxic effects on HeLa cells. Also, this prepared nanocomposite system showed high biocompatibility and low cytotoxic effects in vitro and in vivo (zebrafish embryos model). Hence, the nanocomposite could be used as theranostic agents or cancer diagnostic probes [137,517].

A study conducted by Bankoti et al. used onion peel from cooking waste to synthesize CQDs co-doped with nitrogen, sulfur, and phosphorous. The co-doped CQDs showed stable strong green fluorescence when used for imaging live MG63 and HFFs cells, with maximum emission at a pH of 7–8, indicating its potential for use in biomedical imaging applications. The reported system also exhibited good cytocompatibility, high blood compatibility, high stability against pH, and considerable wound healing activity [137,518].

Manaf et al. used sago bark industrial biowaste to synthesize CQDs via the pyrolysis method. The cell viability results indicated the produced CQDs had low cytotoxicity. Thus, they were used for fluorescence imaging of N2a and melanoma A-375 cells. Due to its safety, it is proposed that a higher concentration of the produced CQD fluorescence probes could be used to image samples that cannot be imaged using low probe concentrations [519].

A study conducted by Cheng et al. reported the synthesis of CQDs from walnut shell biowaste via the chemical cutting method. The obtained CQDs exhibited high photostability, outstanding cytocompatibility, and high ionic strength resistance. The CQDs emitted green fluorescence when used to image MC3T3 live cells. A high ability for intracellular trafficking by only staining the cytoplasm and not the nucleus was also demonstrated [520].

Another study by Cheng et al. demonstrated the use of cellulose-based biowaste, obtained from willow catkin, to synthesize CQDs doped with nitrogen or sulfur. The doped N/S-CQDs showed resistance to high ionic strength, outstanding photostability, excellent fluorescence quantum yield, good biocompatibility, and low cytotoxicity. They also exhibited the ability to detect intracellular Fe3+ ions, leading to quenching of their fluorescence. HeLa cells were used to demonstrate the detectability of the intracellular Fe3+ ions by N/S-CQDS through fluorescence imaging. Upon increasing the Fe3+ ion concentration, the blue fluorescence intensity diminished due to significant quenching. Hence, the obtained N/S-CQDs could be used for labeling intracellular Fe3+ ions in living cells and aid in the detection of any imbalance in intracellular Fe3+, which leads to several diseases [505].

4.4 Au NPs for early disease detection via fluorescence imaging

Due to the increased commercial demand for Au NPs in various applications, more green and sustainable methods have been attempted for their synthesis. One of the prominent approaches to restore this resource-limited material is the recycling of nanowaste and, also, development of nanoparticles synthesis methods depending on the recovered materials. Pati et al. (2016) developed a method to recover gold from nanowaste using α-cyclodextrin. This laboratory-scale strategy successfully recovered gold that was used for the production of Au NPs [521]. A study by Oestreicher et al. recycled aqueous laboratory nanowaste into aqueous HAuCl4. The recovery rate was more than 99% and the recovered gold solution was used in the synthesis of Au NPs through the seed-mediated growth method. This work highlights the completion of a recycling cycle following green chemistry guidelines and considering ecological and economical aspects to achieve sustainability and follow the circular economy approach [522].

Au NPs have great potential in the early detection and diagnosis of diseases, especially cancer. This is due to their outstanding properties. For example, the high fluorescence quenching efficiency of Au NPs is used in fluorescence imaging for switching from on to off states of fluorescence [523525]. In addition, Au NPs are very biocompatible and highly photostable. Au NPs range from single to hundreds of nanometers in size and can be easily functionalized and modified [526]. When excited with a wavelength equivalent to their surface plasmon resonance frequency, Au NPs scatter light resonantly, showing a distinctive optical response [527]. Moreover, Au NPs have outstanding anti-photobleaching behavior when excited by strong light. Although Au NPs have low quantum yields, they strongly display native fluorescence when excited with high energy light [528]. Based on this, fluorescence imaging using Au NPs was developed for cell imaging; the procedures include staining the cells with Au NPs then emitting high energy light, followed by collecting the native fluorescence of Au NPs from cells to develop a cell image [529]. Therefore, Au NPs are a good candidate for the early detection of diseases [483].

A study conducted by He et al. assessed the use of Au NPs as targeted probes for the detection of cancer cells by fluorescence imaging. First, the autofluorescence of HeLa cells was photobleached by strong excitation with light and then Au NP fluorescence was observed. Au NPs were taken in the cells via endocytosis in the differentiation and proliferation phases of the cells. The Au NPs were conjugated to anti-epidermal growth factor receptor antibodies to function as targeted probes for cancer cells, allowing their fluorescence imaging. The fluorescence imaging exhibited high selectivity when compared to other imaging techniques, including dark field imaging. While comparing the Au NPs as a fluorescent probe with other probes, such as QDs and fluorescent dyes, the Au NPs have better potential as a fluorescent probe due to their good photostability, high biocompatibility, ease of synthesis, and ease of functionalization. Hence, as fluorescent probes Au NPs have high potential in targeted drug delivery, cell imaging, and early cancer detection [529].

Au NPs are used extensively in tumor detection. Ultra-small Au NPs are reported to have an enhanced permeability and retention (EPR) effect in tumor sites; they could escape kidney filtration and have a longer half-life in the plasma [530]. A study conducted by Zheng et al. used ultrasmall Au NPs (2.5 nm) functionalized by glutathione (GSH) for fluorescent imaging of mice bearing MCF-7 tumors. The functionalized Au NPs were compared to IRDye 800CW (a small dye molecule) and the results revealed that the Au NP functionalized system had better fluorescence. Moreover, the system showed an enhanced EPR effect and was rapidly cleared from normal tissue after imaging. It has also been reported that the application of GSH–AuNPs is very promising in fluorescent imaging for cancer diagnosis [531,532].

Intracellular pH variations could be used for disease diagnosis. For example, cancer cells deregulate pH intracellularly as they flourish only in an acidic environment [533]. Yu et al. (2016) investigated cellular pH variations through fluorescence imaging. The group developed “submarines” formed from Au NPs that were pH sensitive and functionalized with fluorescent dyes that responded to basic and acidic pH. The submarines showed a great ability to map intracellular pH variations and to pass the blood–brain barrier (BBB). The BBB permeable submarines could be exploited in imaging and treating central nervous system (CNS) diseases, such as adult CNS tumors [534].

Another study conducted by Yu et al. investigated pH-responsive MRI and fluorescence imaging dual-modal Au NPs for tumor diagnosis and imaging. These nanovehicles have the ability for intercellular pH sensing, MRI, and fluorescence imaging of in vivo tumors, and cancer detection due to their modification by the tumor-targeting peptide cyclic arginine–glycine–aspartate (cRGD). Also, it has been reported that these modified nanovehicles could pass the BBB; thus, they could potentially be used in the detection of CNS diseases. To conclude, the developed Au NP based imaging agent, based on sensing pH changes in living cells and determining the size and location of tumors via fluorescence imaging, is a very promising tool for early detection of cancer [535].

4.5 GQDs for early disease detection via fluorescence imaging

GQDs are 0D NPs derived from carbon and consist of at least one G sheet in the nanoscale. Similar to CQDs, GQDs provided high-quality imaging, low toxicity, water solubility, and safe renal clearance with fluorescence emission at the NIR spectral region. Several applications regarding cell motion tracking and tumor imaging with GQDs have been tested. Chen et al. successfully synthesized GQDs to interact with cell surface carbohydrates for tracking cell receptor monosaccharides [536]. After one year, the same group managed to image the hydrogen sulfide level in living cells [537]. Due to the ultra-small size of the GQDs, they can penetrate cell nuclease and have been used for tumor cell detection in vitro. It was reported that GQDs can emit multifluorescent colors, which help detect more than one component within the cell-like emission of red, yellow, and blue fluorescence, allowing multicolor imaging of a glioblastoma U78 tumor cell line in vitro [538]. Similarly, coating GQDs with photoluminescence material has supported multicolor imaging inside the HeLa cell line in vitro [539,540]. Additionally, GQDs showed high selectivity and specificity for detecting more cell lines in vitro, including the Schwan cell line rsc96 [541] and murine alveolar macrophage cells (MH-S) [509].

In cancer detection applications, GQDs have been combined with well-known biological NPs, like IO NPs, to enhance the detection of carcinogenic HeLa and MCF-7 cell lines in vitro [542]. Similarly, GQDs were combined with fluorine for detecting HepG2 cells within a 3D model structure, mimicking the tumor microenvironment of these cells [543]. From this point, bioimaging in vivo has begun. Initially, GQDs were injected intravenously, subcutaneously, and intramuscularly in nude mice to evaluate the bioimaging of biological components in vivo as well as the biosafety of GQDs [509,540,541]. Furthermore, GQDs have been reported to have the potential for targeting tumor cells inside mice models. Nurunnabi et al. evaluated carboxylated GQDs cytotoxicity in addition to detecting the KB tumor of mice models [544]. Also, the targeting of reactive oxygen species (ROS), as a tumor biomarker of a pancreatic cancer cell line (PANC-1) injected inside a nude mice model, by synthesized cyclotriphosphazene-doped GQDs (C-GQDs) has been reported [545]. These results gave hope for treating cancer cells with more accurate drug delivery by targeting only tumor cells rather than normal cells [499,546]. Huang et al. managed to introduce folate–GQDs as an anti-cancer treatment for human liver carcinoma (HepG2) and human cervical (HeLa) cancer cell lines in vitro by injecting folate–GQDs inside zebrafish embryos to assess cytotoxicity [547]. Yao et al. used a combination of mesoporous silica NP GQDs (GQD–MSNs) using DOX as chemical – a photothermal drug for targeting the 4T1 breast cancer cell line [548]. Joshi et al. introduced sliver–GQDs loaded with inulin as a cancer therapy into pancreatic cancer cells in vitro and in vivo [549].

Biomass wastes originate from living organisms that contain carbon atoms as their major chemical element. For example, fossils, coal, petroleum, and natural gases release CO2 when burned. Interestingly, CQDs successfully synthesized from biological wastes have been used in several bioimaging applications. For example, Atchudan et al. created recycled CQDs from banana peel waste and used them for bioimaging in nematodes [550]. Anthony et al. recycled CQDs from rice wastes and imaged A549 cells in vitro and in vivo (injected inside rat models) [551]. Although the synthesis of GQDs from biological wastes is rarely reported, some successful attempts have been established [184]. In 2018, Ding et al. synthesized GQDs from lignin biowaste and introduced them to RAW 264.7 cells (monocytes/macrophage-like cells) for bioimaging [552]. Likewise, Zhang et al. synthesized nitrogen-doped GQDs (N-GQDs) from the marigold plant for detecting Fe3+ ions as a target for bioimaging inside living cells [553].

4.6 Magnetic imaging

The application of novel diagnostic tools in biomedical sciences enables early diagnosis of many diseases, such as cancers [554] and Alzheimer’s disease, which may help to ensure appropriate therapy, delay disease progression [555], and limit complications [556]. This would imply intensive development of different molecular imaging techniques [557] and medical diagnosis, including medical imaging [483], which allows identification of anatomical structures, as well as molecular and cellular imaging [558]. These techniques are classified as low and high magnetic field techniques, including MRI [559], which represents one of the medical imaging modalities widely used in detecting many diseases, like rheumatoid arthritis while differentiating it from other inflammatory arthropathies [560].

MRI is one of the most powerful diagnostic methods for in vivo molecular imaging through non-invasive prediction of diseases at the molecular level. This allows visualization of the molecular characteristics of physiological or pathological processes, without invasive procedures, in living organisms before they manifest in the form of anatomic changes [561]. MRI is based on the features of hydrogen nuclei preceding an applied magnetic field. The relaxation processes, through which the nuclei return to their original aligned condition, can be taken advantage of with the application of a radiofrequency pulse and magnetic field gradients [562564]. Nevertheless, the resolution and imaging sensitivity of MRI relies heavily on the use and performance of metallic CAs [563]. Three categories of MRI CAs have been distinguished. The first is T1-weighted CAs, wherein most medical agents belong and confer a positive contrast (i.e., paramagnetic materials) [565]. T2-weighted CAs, which shorten the T2 relaxation time and confer a dark contrast (i.e., superparamagnetic iron oxide) [566], have been widely used as MRI CAs to detect cancer [567]. Dual-weighted contrast, the third category, shortens both T1 and T2 relaxation times [568]. MRI presents advantages over the other medical imaging techniques thanks to its high resolution, deep penetration [569], efficient intrinsic contrast [570], and its ability to image soft tissues [571].

Although its applications are vast, magnetic imaging modality lacks specificity, which may leads to false-positive results [572]. It also presents technological, physical, financial, and safety limitations [573 as well as bulky instruments [574] and inhomogeneity of the magnetic field, which may result in non-homogeneity in image signals [575]. To overcome some of these disadvantages, the application of NMs in medical imaging can help minimize detection limits [576] and increase sensitivity through the generation of efficient interaction of molecules with signal generating particles [577]. Compared to bulk materials, NMs provide more advantages due to their magnetic susceptibility [578], finite sizes, and the magnetic behaviors of particles. Magnetic NPs (MNPs) have demonstrated wide applications as CAs that enhance the MRI signal and image quality and present different characteristics, like superparamagnetism [557], that provide more magnetization [558]. Depending on their medical applications, MNPs are divided into paramagnetic, ferromagnetic, and superparamagnetic particles, which impact MRI contrast differently and have different core sizes and shapes that define their magnetic properties [579].

Recently, more attention has been given to the development of new NMs, such as QDs and MOs, for the diagnosis and/or treatment of various diseases [580]. Here, we cite some of the NMs, as shown in Figure 13, used with MRI for the early detection of diseases.

Figure 13 
                  Schematic representation of some NPs recycled from wastes and used in MRI for the diagnosis of diseases, especially tumors.
Figure 13

Schematic representation of some NPs recycled from wastes and used in MRI for the diagnosis of diseases, especially tumors.

4.7 Magnetic iron oxide

Magnetic iron oxide has unparalleled properties, such as its interaction with magnetic fields and field gradients. These properties enable magnetic separation, improvement, and recycling of MNPs, as well as the tracking and visualization of the local MNP environment and labeling of cells through MRI. Yan et al. found that iron oxide (Fe3O4) MNPs exhibited an intrinsic peroxidase mimicking activity. Moreover, the enzyme sensitivity of Fe3O4 measures the enzyme activity of proteases, methylases, and restriction endonucleases [561,581]. For in vivo tumor imaging, MNP probes could be delivered to tumors by either a passive or active targeting mechanism. In the passive mode, macromolecules and nanometer-sized particles have been accumulated preferentially at tumor sites through EPR effects. This effect is believed to arise from two factors. The first factor is antigenic tumors, which produce vascular endothelial growth factors that hyper permeabilize tumor-associated neo-vasculatures and cause leakage of circulating macromolecules and small particles. The second factor is that tumors decrease the effective lymphatic drainage system, which leads to a subsequent macromolecule or NP accumulation. Passive tumor targeting requires MNP probes to have long plasma circulation times, which are typically achieved by shielding the MNPs with polymers, such as polyethylene glycol (PEG) and dextran. PEG and dextran are hydrophilic polymers with low immunogenicity and can help NPs escape uptake by the reticuloendothelial system (RES) [561,582584]. Radionuclides, such as 18F or 64 Cu, have been loaded to surface-limited organic ligands on MNPs for tumor diagnosis [580]. Lai et al. covered MNPs with an iridium complex that reacted with silane and combined them with tetraethyl orthosilicate. The final mixture was hydrolyzed over the NP surface. This multimodal system was used for phosphorous labeling and, at the same time, for apoptosis of cancer cells induction by synthesis of O2 [580,585].

4.8 Superparamagnetic IO NPs (SPIONs)

SPIONs are the most widely used NMs in clinical MRI [586], where they have shown remarkable enhancement in sensitivity [587]. These NPs can be functionalized and adapted to different soft tissues for paramagnetic agents [588]. SPIONs have presented the unique biological property of uptake by macrophages during the inflammatory response. This property could present advantages for visualizing several affllictions indirectly using MRI [589], such as atherosclerosis [590], myocarditis, and several kinds of infections [591]. SPIONs were effective as negative CAs due to their ability to decrease the transverse relaxation of tissue water protons and enhance the relaxivity (r 2) value. Different T2 CAs (i.e., magnetic ferrites CoFe2O4 and MnFe2O4) have been used as a T2 due to their superior properties in enhancing the distinction between healthy and infected tissues [592594].

SPIONs are characterized by low toxicity, but they present difficulty in being distinguished from other iron-rich tissue [595,596] that would interfere with the biological iron metabolism [597,598]. On the other hand, these MNPs present an instability problem. This could be remediated by the application of surface coating, which could decrease their potential toxicity, increase their efficiency, as well as control their size and limit their accumulation [599]. Feridex®, an example illustrating this procedure, is a commercialized medical product used for the detection of liver lesions and identifying abnormal hepatic cells. The principle of this product is based on the uptake of the SPIONs [595] and biocompatible NPs that can be recycled using simple magnets [600] with phagocytic kupffer cells located in the RES. These cells are absent within malignant liver cells. This would create a signal intensity difference between normal and abnormal cells, hence generating a difference in contrast when visualizing using MRI [595]. Another study realized by Lindemann et al. presented dextran-coated SPIONs as innovative tracer material for tumor cell analysis in MPI [601]. This MPI presented better sensitivity than MRI and used an oscillating magnetic field that served to generate the signal derived from MNPs [602].

The use of intraprostatic injections of SPIONs by MRI is safe and efficient in the identification of sentinel lymph nodes for prostate cancer detection [568]. The conjugation of the chitosan-coated MNPs and of surviving antisense oligonucleotides to formulate survivin-targeted NPs could be used with MRI for pancreatic tumor detection [572].

4.9 Cellulose nanocrystals (CNCs)/Fe3O4 NPs

The use of CNCs/Fe3O4 nanocomposites has attracted great attention because of their current and potential ability as dual T1–T2 CAs for MRI [603]. CNCs are a type of cellulose NM that act as dual CAs because of their advantages, such as nontoxicity, large surface area, low price, high mechanical strength, and stiffness [604,605]. Moreover, they have been used in biomedicine, tissue engineering, and biosensors [606]. CNC/Fe3O4 nanocomposite for Pickering emulsions based on ultra-small Fe3O4 NPs and CNC–poly citric acid (CNC–PCA) nanoplatforms have been investigated as dual magnetic CAs [603]. The results of in vitro cytotoxicity tests on HeLa cell lines at 24 and 48 h revealed compatibility and low cytotoxicity (up to 200 μg mL−1 Fe). In vitro, the MR relaxivity ratio (r 2/r 1) of CNC–PCA/Fe3O4 nanocomposites was calculated to be 7.0. Consequently, these novel composites have potential for MRI applications as dual CAs for the early detection of disease.

4.10 Au NPs (magnetic/gold non-hybrid particles)

Au NPs are an exciting class of NMs that can be recycled from various types of wastes, such as wastes using microorganisms (biometallurgy) [607] and food wastes [329,334]. Au NPs could be used for various biomedical uses, including bioimaging, because of their bioinertness, surface chemistry controllability, X-ray opacity, and optical features [608,609].

A green chemistry process using grape seed proanthocyanidin as a reducing agent has been used to produce crystalline magnetite/gold nanohybrid particles (∼35 nm in size) from a single iron precursor (FeCl3) [608,610]. The hybrid Fe3O4 compound showed superparamagnetization with dark T2 contrast (124.2 ± 3.02 mM−1 s−1) from MRI and magnetization analysis. Moreover, phantom CT imaging showed sufficient X-ray contrast due to the presence of nanogold in the hybrid component. Given its possible use for stem cell monitoring and imaging, compatibility assessment was carried out on human mesenchymal stem cells. The serial optical parts of the cells incubated with NPs showed that the particles were distributed after they were taken up. Moreover, even at a high concentration of 500 μg mL−1 and incubation up to 48 h with no apoptotic signals or ROS formation, strong biocompatibility was observed. This is in line with the outcomes of cytotoxicity experiments and can be considered strong evidence that the biocompatibility of the diagnostic nanoprobe is valid [608]. Considering the described properties of Fe3O4 and Au NPs, it seems that mixing both NPs in a single nanocomplex may have potential in the fields of cancer diagnosis and therapy [611].

4.11 PEGylated iron-oxide–gold core–shell NPs

PEG-coated Fe3O4 NPs produced to date are too large to enter pancreatic tumors as they have insufficient circulation in the blood compartment [612,613]. Recently, superparamagnetic gold-coated core–shell NPs have been considered very important in biomedical applications [613618]. NPs with Au and iron oxides are considered biocompatible and have been widely used in both optical and magnetic applications. In addition, a gold layer on NPs was found to be stable under biological conditions [611,613,619].

Kumagai et al. worked on developing PEG-coated iron-oxide–gold core–shell NPs (PEG–AuIONPs) for use as a T2-weighted MRI CA for pancreatic tumor model imaging. Their findings showed that PEG–AuIONPs have extended circulation in blood and improved the MRI of models of subcutaneous colon and pancreatic tumors. These results indicate that PEG–AuIONPs are a successful way to develop MRI CAs for the diagnosis of many tumor groups, for example, pancreatic cancer. By using their method, precise control of hydrodynamic size and efficient PEG density on the AuIONPs was achieved [613].

4.12 Carbon NPs

CNMs have shown wide applications in biomedical tumor imaging due to their optical and magnetic properties. CNTs and G are some of the CNMs used due to their structural and physicochemical properties [620] as well as for their ability to be functionalized [621]. These two agents could be used in biomedicine as nanocarriers [622] for cancer theranostics, which combine both diagnosis and therapy [623,624]. A research study has been carried out to develop a GO and gadolinium (Gd3+) complex for use as a theranostic agent. This was achieved through the conjugation of diethylene-triamine-penta-acetic acid with GO and complexing it with Gd3+ followed by loading the surface of the GO with DOX, an anti-cancer drug. The formed complex showed better contrast imaging ability than Gd3+, abased T1 CA, and DOX was released successfully during the chemotherapy [625].

The conjugation of GO–Fe3O4 could be utilized as a CA for magnetic imaging [626]. Another study referred to the conjugation of amino dextran coated Fe3O4 NPs to GO. This hybridization showed an enhancement in the MRI detection of human cervical cancer compared to Fe3O4 NPs alone [627]. From another context, a research study succeeded in covering magnetic single-walled carbon nanotubes (SWCNTs) with magnetic Fe3O4 NPs and coating them with multilayer polyelectrolytes, which were then linked covalently to FA as a targeting agent. The in vitro results showed an enhancement in the MRI for human cervical cancer HeLa cells [628]. Another in vitro study related to the enhancement of single-walled carbon-NPs magnetic targeting properties through MRI used Fe3O4 tagged SWCNTs to enhance its sensitivity for the detection of 4T1 induced breast cancer in murine. The results showed efficient and safe employment of the MRI signals for cancer cell detection, which encourages further studies utilizing this nanocarrier for other biomedical applications, including diagnosis and drug delivery [629].

4.13 GO NPs

GO has huge potential for integration in biomedical applications as it is a most promising NM among the carbon family for efficient multifunctional theranostic agents. GO has high bioavailability and biocompatible properties in biological systems. Also, it is photothermal, magnetically thermal, paramagnetic, hydrophobic, and has low cytotoxicity. To enhance the biocompatibility of CAs and improve the MRI capabilities of Fe3O4, GO–Fe3O4 has been synthesized in conjunction with SPIONs and GO. This succeeded in improving physiological stability, cellular MRI, and decreased cytotoxicity [517,630632]. Moreover, GO–Fe3O4 with SPIONs helped overcome side effects, such as heart failure, aggregation in the skin, kidneys, and brain, which may lead to kidney disease and nephrotic system fibrosis, common in other MRI CAs, such as Gd3+ or Mn2+ [633,634].

4.14 CDs

CDs include carbon nanodots, CQDs, quantum graph dots, and carbonized polymer dots [635]. Biomass is a good source for the production of CDs due to its abundance, availability, environmentally friendly nature, and being a source of low-cost renewable raw substances [137]. Biomass is an abundant, complex, heterogeneous, biodegradable, and bioorganic material that can be collected from various sources including perennial grass, organic domestic waste, agricultural residues, poultry, fishery, forestry, and related industries. Natural organic biomass waste is primarily made up of cellulose, hemicellulose, lignin, proteins, ash, and some other ingredients [137,636,637]. Xu et al. synthesized CQDs from apple juice [638,639]. CDs from Trapa bispinosa peel were prepared by Mewada et al. and showed low cytotoxicity and good biocompatibility in Madin–Derby canine kidney cells. Hence, they are promising for use in biomedical applications [137,640].

There are two methods for adapting CDs for the improvement of MRI CAs: (1) incorporate Gd3+ or Mn2+ in CDs for T1 contrast enhancement [517,641] and (2) hybridize CDs with IO NPs for T2/T2* contrast enhancement [641643]. Using natural chemical exchange saturation transfer (CEST), the MRI contrast properties of metal-free CDs could be utilized to create contrast without (super)paramagnetic labels. This is in contrast to paramagnetic metals that might present toxicity problems or the CD/iron oxide combination, which could present undesirable outcomes. CDs, with their favorable size and biocompatibility properties, are appealing diamagnetic CEST CAs. These agents have been used for a wide range of biomedical applications, such as tumor screening and cancer cell theragnostics [639,644,645], or are used as specific markers for tumor vasculature [641,646]. Besides iron oxides, both fluorescence and ferromagnetic properties were shown in the transition metal ion doped CDs. Ji et al. have synthesized Mn-doped CDs (Mn-CDs) that presented clear MR imaging abilities of the brain glioma area after 30 min and 2 h [645]. Moreover, Pakkath et al. produced TM2+ doped CDs (Mn2+, Fe2+, Co2+, and Ni2+) and applied them as T1-weighted contrasts. Upon injection of 10 mL TM2+ doped CDs into zebrafish, in vivo fluorescence and magnetic imaging showed that the TM-doped CDs were suitable agents for T1-weighted contrast with bright green emission at administrable amounts [646]. Although these magnetic characteristics are too poor to apply to MRI, this indicates a new path for the combination of optical and magnetic properties. A composite of IO NP doped CDs (IO-CDs) provides both fluorescent and magnetic capabilities. These properties could be used for MRI/fluorescence multimodal bioimaging. IO-CDs are characterized by low cytotoxicity and good fluorescence imaging ability and could be potential T1/T2 CAs and efficient fluorescent biomarkers for in vivo magnetic fluorescence/resonance imaging [635,647].

4.15 ZnO NPs

Due to their biodegradable properties in biological media, both ZnO NPs and aluminum-doped ZnO (AZO) NPs have been used for biomedical applications such as monitoring tumor progression by MRI, delivering substances through the gut barrier, and surgery. On the other hand, AZO NPs can be a non-degradable matrix and, therefore, might be used for their biostability properties in fluorescence-directed biopsy [648]. A ZnO matrix doped with foreign ions has luminescence properties. These nanocomposites could be used in biomedical applications thanks to their phonons, efficient excitation, and emission properties in the visible region [649]. Gd-doped ZnO QDs, a ZnO nanocomposite containing Gd3+ ions, can decrease the time of longitudinal (T1) relaxation of water protons with bright contrast at its location. These QDs and ZnO have weak toxicity, and the nanocomposites were effective in biomedical imaging for in vitro MRI [650]. In a study related to the functionalization of NMs, Gd-doped ZnO QDs nanocomposites were formulated (with sizes <6 nm) for both optical and MRI owing to the direct relationship between the emission intensity of the Gd-doped ZnO QDs and the concentration of Gd3+. Remarkable maximum emission intensity was observed at 550 nm. Surface coating of Gd-doped ZnO QDs with N-(2-aminoethyl)aminopropyltrimethoxysilane showed low toxicity to HeLa cells and the ability to enhance imaging quality for in vitro visualization of HeLa cells with both confocal microscopy and MRI [651].

4.16 Biosensors

There are biological markers that need frequent and continuous measurement. Traditional methods for biomarker detection are costly, time consuming, and need complex devices and experts to work devices. The use of biosensors with nanotechnology has been one of the best biomedical applications for the rapid and accurate diagnosis of disease as appropriate treatment can be given at an early stage reducing the mortality rate [652].

Biosensors are high-sensitivity analytical devices that have become an essential part of our modern life because they provide precise monitoring of our bodies and the surrounding environment. Biosensors, a hybrid of biological elements and physicochemical components used to detect particular biological molecules or biomarkers of a medium and generate a measurable signal (usually a voltage), analyze the biological response of living organisms [653,654].

The first biosensor was designed by the biochemist Leland Clark, who is called the father of biosensors, in 1950 [655]. The term “biosensor” was coined in 1977 by Karl Cammann [656] and consists of two terms: the term “bio” is short for “biological response” and the term “sensor” originates from the Latin word “sentire,” which means “to feel or to identify” something [657]. Biosensors are characterized as highly sensitive, highly specific, and easy to use analytical devices. In principle, the biosensing technique consists of three fundamental components: receptor, transducer, and reader device. These components measure the physical or chemical changes in the element or biological marker to be measured. A receptor, which is a biological element, senses the physical or chemical stimuli and transforms them into electrical energy, wherein the generated electrical energy depends on the type of biological element. The transducer performs the function of converting this energy into an analytical signal, which can be analyzed and presented in an electronic form that is transmitted to the reader device. The reader device consists of an amplifier, conditional filter circuits, and a display unit, which further implement the detection response and represent it as a numerical value [652,658].

Biosensors are classified according to the parameter that is measured by the physicochemical transducer of the biological biomarkers, such as optical, electrochemical, acoustic, and thermal [659]. In the last few decades, biosensors have been widely used for the detection of several components including gases, metabolites, pollutants, microbial load, and other organic compounds, and in a wide range of biological applications such as food analysis, detection of biomolecules that are either an indicator of a disease or target of a drug, as clinical tools to detect diabetes, and to monitor protein fragments that are basic cancer biomarkers. Scientists anticipate that, in the near future, we could detect several diseases, such as diabetes, airborne diseases, and cancer, at a very early stage to provide a good chance of treatment [660,661].

4.17 Early detection of diabetes

Diabetes is a common disease that strikes different age groups, the young, the elderly, and even children, and requires periodic, rapid, and accurate analysis of glucose level to keep it at normal levels [662]. Electrochemical biosensors have contributed to the rapid evolution of glucose level monitoring in blood. Enzymatic biosensors are traditional electrochemical glucose biosensors that use glucose oxidase enzyme (GOx) as a catalyst to oxidize the glucose at the electrode, producing gluconolactone, H2O2, and electrons [663,664]. The generated H2O2 and electrons are related to the glucose concentration in the sample. Limitations of this technique include some difficulties in handling, short storage life, and being easily affected by temperature and chemicals, which prevent accurate early detection of high blood glucose levels.

Nanostructured materials have been utilized to produce electrochemical non-enzymatic biosensors to overcome the above-mentioned challenges, receive an accurate record of glucose levels, obtain stability and reproducibility, and form nanozymes on the surface of the electrode that offer several advantages in the detection of glucose, such as simplicity, low cost, long storage life, and high selectivity/sensitivity [664,665].

In enzyme-free glucose biosensing, CuO and CD nanocomposites have been used as nanozymes with unique properties, such as enhanced surface area and improved electrode sensitivity. CuO NPs have been used as a catalyst because of their low cost, facile preparation, low toxicity, and notable electrochemical catalytic properties [666]. Moreover, CDs composed of CNPs with diameters of less than 10 nm, high surface area, and chemical stability could improve sensing sensitivity due to the enhanced electron transfer characteristics associated with CuO NPs and increased electrode surface area. This makes non-enzymatic electrochemical biosensors effective in the early detection of diabetes [667,668]. Mehrab et al. proved that recycled CuO could be used effectively and repeatedly as nanocatalysts with notable electrochemical catalytic properties, low cost, facile, and non-toxic preparation [667]. Nanocomposites of recycled CuO nanocatalysts and CDs merge the advantages of both recycled NPs and could be used effectively for the detection of diabetes at early stages [669,670].

Ahmad et al. (2017) fabricated non-enzymatic glucose detecting electrodes using ZnO nanorods (NRs) grown vertically on fluorine-doped tin oxide (FTO) electrodes. The electrodes were then decorated by CuO NPs to enhance the stability and efficiency of the CuO–ZnO NR/FTO electrode. In addition to improved reproducibility and anti-interference, the electrodes were able to be reused more than five times. The response of the sensor was found to range from 93 to 97% of the original response [671].

Several NPs recycled from different sources of waste have been utilized as biosensors for the early detection of different diseases, as illustrated in Table 13. Recycled Fe3O4 MNPs were utilized in electrochemical biosensors owing to their low biotoxic effect, biocompatibility, and strong superparamagnetic properties [672]. Li et al. revealed that recycled Fe3O4 NPs could be used as a NP-based catalyst qualified for recycling more than eight times while maintaining a high level of operation without any significant losses in activity [673]. Zhang et al. incorporated Fe3O4 NPs with synthesized nitrogen-containing chitosan-doped G (CG), wherein chitosan improved the biocompatibility of the electrode and provided a suitable environment for enzyme immobilization. This combination increased catalytic activity, provided a larger active surface area, and enhanced the transportation of electrons, which enabled Fe3O4/CG to exhibit high-performance catalytic activity as electrochemical biosensors for the detection of glucose in blood [674676].

Table 13

NPs recycled from different sources of waste and utilized as biosensors for the early detection of different diseases

NP Usage Advantage Signal transduction Limitation Source Ref.
CuO Detection of glucose in the blood Recyclability Electrochemical Vegetable waste [666]
Selectivity
Low cost
Chemical stability
ZnO Detection of glucose in the blood Reproducibility Electrochemical Complex fabrication process Zn–C and Zn–MnO2 batteries [671,701]
Anti-interference
Recyclability
Fe3O4 Detection of glucose in the blood Recyclability Electrochemical Easy aggregate Steel industry waste [672,702]
Low toxic effect
High oxidization probability
Biocompatibility
Strong superparamagnetic property
NGO Aptamers, DNA or RNA biosensors Low cost Electrochemical Hard to dissolve in water Agricultural waste [683]
High yield production
Distinctive physicochemical properties
CNTs Early cancer diagnosis High conductivity Electrochemical, optical Need to functionalize the surface Polymer waste [683]
Large surface area
Fast electron transfer
Irreversible agglomerates in aqueous solution
High mechanical strength

4.18 Early detection of cancer

Cancer is the second leading cause of death in the world [677]. Early diagnosis of cancer is crucial to increase the chances of survival and provide more affordable treatment [678]. Recycled NP biosensors have shown high efficiency in the early detection of different cancers where current diagnostic methods failed [679]. Biosensors manufactured from RNMs are designed with many binding sites that capture various tumor biomarkers. Various CNMs have been used in the development of biosensors as they offer biocompatibility, high specific area, and excellent optical, electrical, and mechanical properties [680].

Two-dimensional nano-GO (NGO) conjugated with an aptamer biosensor showed high sensitivity and selectivity in the early stage detection of the main types of cancer biomarkers [681]. NGO chemical properties allow the formation of many covalent and non-covalent bonds with other NP, polymer, and biological entities [682]. From an industrial approach, NGO has low cost, high production yield, and distinctive physicochemical properties that present great potential in biology [683], as shown in Table 13. Aptamers, single-stranded nucleic acid particles, DNA or RNA, attach to NGO instead of antibodies because of their easy synthesis, low cost, low immunogenicity, and low variability empower. Upon conjugation to the NGO, aptamers act as exchangeable building blocks for functionalizing CNMs, which facilitates their clinical application [681]. Tan et al. designed a probe using NGO and carboxyfluorescein-labeled Sgc8 aptamer (FAM-apt) to detect CCRF-CEM cells (human acute leukemic lymphoblast cell lines) based on the fluorescent quenching property of NGO [684]. Their probe can isolate CCRF-CEM cells from a peripheral blood sample that contains target and non-target cells suffering from acute lymphocytic leukemia. When the aptamers are adsorbed to the NGO surface by π–π stacking, the fluorescence of the FAM-apt is quenched when there are no target cells as the NGO and the fluorophore are too close to transfer energy. In case CCRF-CEM cells are detected, the weak binding force of the NGO–aptamer allows the aptamer to fall off the NGO surface and bind to the cells, causing fluorescence. In the absence of the cells, the aptamer is still connected to the NGO with no fluorescence to restore. The more CCRF-CEM cells found, the higher the fluorescence intensity. In addition to CCRF-CEM cells, NGO–aptamer has the potential to detect early other cancer cells, such as Ramos cells, H22 cells, and 293T.

Multi-walled carbon nanotubes (MWCNTs) have also been used to develop biosensors. Berkmans et al. have developed the rotating cathode arc discharge technique to create MWCNTs from PET waste [685]. This method recycles PET mineral water bottles and creates MWCNTs in the cathode, paving the way for the manufacture of biosensors. Moreover, Singh et al. have developed MWCNT biosensors that detect aflatoxins in the body related to the early diagnosis of cancer [686]. The International Agency for Research on Cancer has categorized B1 aflatoxins as a group one carcinogen, while G1, G2, and B2 aflatoxins are group two carcinogens [687]. These materials are found in many agricultural products and have mutagenic and carcinogenic effects [688]. Liver cancer is most prevalent in people affected by aflatoxins, even in small concentrations [689]. Hence, the early detection of aflatoxins in the body helps either prevent the primary occurrence or avoid the reoccurrence of cancer. The MWCNT electrochemical-based biosensor will help in detecting aflatoxins because of its captivating properties such as high conductivity, large surface area, fast electron transfer properties, biocompatibility, and high mechanical strength. MWCNTs have been treated using nitric/sulfuric acid solutions to form carboxylated MWCNTs (c-MWCNTs) that form covalent bonds with anti-aflatoxin B1 antibodies (anti-AFB1). Then, the c-MWCNTs are deposited onto an indium tin oxide substrate using the electrophoretic deposition technique to give it electrochemical sensation. The anti-AFB1/MWCNT/ITO bioelectrode showed sensitive detection of aflatoxin B1; the electrode current increased when the concentration of aflatoxin B1 antigen increased [686].

Au NPs have played an important role in the evolution of biosensors. Their electronic, magnetic, optical, physical, and chemical properties make them great sensing material. They are noble, biocompatible, their shape and size can be easily tuned, and their surfaces can be easily functionalized [690]. However, the production methods of Au NPs are based on the use of reducing agents, which are toxic and considered a human health threat in addition to their environmental pollution burden. Another traditional method depends on the breakdown of Au NPs, which requires a lot of energy and negatively affects the environment. A green method was developed to biosynthesize Au NPs from plant tissue extract and different plant parts, including leaf, bark, stem, and root [691]. This extract was simply treated with auric salt solutions, which helped to separate the Au from the extract and change it to NPs. Then, the Au NPs could be obtained by centrifugation for use in many biomedical applications, including biosensors [692].

4.19 Early detection of Parkinson’s disease (PD)

Recycled waste materials, such as Au NPs and SWCNTs, have been involved in the manufacture of biosensors for the early detection of PD [693]. PD is a neurodegenerative disorder where brain neurons die, especially in the Substantia nigra area, with a high incidence in elderly people [694]. Following the death of nerve cells, Lewy bodies are the surviving lesions found in PD-affected persons. The early diagnosis of PD is important for prompt and effective treatment using neuroprotective therapeutics to avoid complete loss of the substantia nigra of dopaminergic neurons [695].

In a study conducted by Zhang et al., SWCNTs seeded with Au NP–urchin conjugated antibodies on an interdigitated electrode (IDE) was developed and had high performance in detecting α-synuclein [693]. SWCNTs were used to act as an attractive NM due to its high-affinity molecular recognition, biocompatibility, and higher level of fluorescence quantum efficiency [696]. SWCNTs are mainly used in electrically based applications as their electrical signals reflect the movement of biomolecules and their interactions with the biosensor [697]. Au NPs have easy functionalization and excellent optical properties, in addition to their good conductivity, biocompatibility, and catalytic properties [698]. Sea urchin-shaped Au NPs were used either on the surface to conjugate the capture molecule or to immobilize the target [699]. An IDE has been fabricated with nanocomposite on silica. This IDE sensor was designed with a dielectrode, uniformly arranged fingers, and gaps that cannot be modified and where molecules can be assembled to transduce current [700].

5 Role of RNMs in the treatment of diseases

5.1 Antimicrobial activity

A key biomedical application of NPs is their use as innovative antimicrobial agents, as shown in Table 14, which overcomes the drawbacks of conventional antimicrobial drugs [703]. NPs have diverse mechanisms of action to kill pathogenic microorganisms, such as oxidative stress and metal ion release [704]. It has been proven that the smaller the particle size, the better the antimicrobial activity [705].

Table 14

Application of recycled NPs as therapeutic antimicrobial agents

NM Biomass sources Applications Ref.
Au NPs Watermelon rind Antibacterial activity against Escherichia coli, Bacillus cereus, and Listeria monocytogenes [335]
Au NPs Citrus maxima peel Antibacterial activity against E. coli and Staphylococcus aureus [333]
Au NPs Allium noeanum leaf Antibacterial activity against E. coli, Streptococcus pneumoniae, Bacillus subtilis, S. aureus, Staphylococcus saprophyticus, Salmonella typhimurium, Pseudomonas aeruginosa, and Shigella flexneri [731]
rGOX Chenopodium album Antibacterial activity against S. aureus and E. coli [710]
AC Bamboo charcoal Antibacterial activity against coliform bacteria and Salmonella [712]
AC Kitchen soot Antibacterial activity [713]
CNMs Rapeseed oil cake Antibacterial activity against S. aureus, Pseudomonas diminuta, Yersinia enterocolitica, Salmonella enterica Typhimurium, Candida albicans, and E. coli [707]
CNFs Electrospun biomass using biomass tar and silver NPs Antibacterial activity against E. coli and S. aureus [709]
G Tridax procumbens leaf Antibacterial activity against E. coli and S. aureus [711]
CuO NPs Aspergillus niger Antibacterial activity against E. coli, S. aureus, Klebsiella pneumoniae, Micrococcus luteus, and B. subtilis [715]
Cu NPs Cissus arnotiana biomass Antibacterial activity against E. coli [716]
CuO NPs Camellia sinensis leaf biomass Antibacterial activity against K. pneumoniae and S. aureus [717]
ZnO NPs Punica granatum fruit peel biomass Antibacterial activity against E. coli and Enterococcus faecalis [718]
ZnO NPs Tabernaemontana divaricata leaf Antibacterial activity against E. coli and S. aureus [719]
Iron NPs Citrullus colocynthis pulp and seed biomass Antibacterial activity against B. subtillis, S. aureus, E. coli, and P. aeruginosa pathogenic bacterial strains, and moderately inhibited C. albicans [721]
Iron NPs Azadirachta indica (neem) leaf Antibacterial activity [724]
Iron NPs T. procumbens leaf Antibacterial activity against P. aeruginosa [725]
Iron NPs Kappaphycus alvarezii Antibacterial activity against E. coli and S. aureus [726]
Iron NPs Mimosa pudica root Antibacterial activity [722]
Iron NPs Dodonaea viscosa leaf Antibacterial activity against E. coli, B. cereus, S. aureus, K. pneumoniae, P. fluorescens, B. subtilis, and L. monocytogenes [723]
Iron NPs Eucalyptus robusta leaf Antibacterial activity against S. aureus, P. aeruginosa, and B. subtilis [727]
TiO2 NPs Plum, peach, and kiwi fruits Antibacterial activity against E. coli and B. substilis [228]
TiO2 NPs Artemisia haussknechtii leaf biomass Antibacterial activity against E. coli [730]
TiO2 NPs Morinda citrifolia leaf biomass Antibacterial activity against E. coli [728]
CQDs Lactobacillus plantarum biomass Antibacterial activity against E. coli [733]

CNMs, such as CNFs, G, AC, and CNTs, can cause membrane damage in bacteria owing to oxidative stress and other modes of action [706]. CNMs synthesized from rapeseed oil cake, which is an industrial bulk waste byproduct produced during the oil extraction process, can prevent the growth of Staphylococcus aureus, Pseudomonas diminuta, Yersinia enterocolitica, Salmonella enterica Typhimurium, Candida albicans, and Escherichia coli [707].

CNFs killed methicillin-resistant Staphylococcus epidermidis after 2 h of direct contact [708]. The antibacterial effect of CNFs from electrospun biomass using biomass tar and silver NPs has been confirmed [709]. This result can be explained by the disruption of the bacteria membrane or the oxidative stress process [708], as shown in Figure 14. Moreover, GO, especially rGO synthesized from biomass sources, has shown superior antibacterial activity [710]. Furthermore, biomass-synthesized G from the leaf extract of Tridax procumbens has shown antibacterial potential against both gram-positive and gram-negative bacteria through the interaction of G with the microbial cell; they connect to the cell surface, causing cell membrane disruption and oxidative stress [711].

Figure 14 
                  General mechanisms for antimicrobial action of NPs.
Figure 14

General mechanisms for antimicrobial action of NPs.

rGO using Chenopodium album demonstrated efficacy against S. aureus and E. coli [710]. The minimum inhibitory concentration (MIC) of rGO against both bacteria strains was 125 µg/mL, unlike conventional GO, which had a MIC value of 250 µg/mL [710]. This reflects the benefits of the biomass-derived reduction method versus other synthesis methods. The suggested rGO mechanism of action is disruption of the bacteria cell wall or cytotoxicity through oxidative stress formation [710]. Another antimicrobial agent from biomass-synthesized CNMs is AC. Charcoal from bamboo sources significantly reduced the counts of coliform bacteria and Salmonella while increasing the level of beneficial fecal anaerobic bacteria [712]. Furthermore, AC NPs produced from kitchen soot, which is a carbon-rich byproduct of the combustion process, are antimicrobial as well [713]. AC can penetrate the bacteria cell membrane and then interact with intracellular sites, which leads to cell division inhibition and, consequently, cell death [713].

CNTs are considered ideal antimicrobial agents due to their small diameter and higher surface area [714]. CNTs begin their effect by first connecting to the microorganisms and then disrupting their cellular membrane and morphology [714]. They also prevent DNA replication and generate ROS [714]. CNTs showed antibacterial efficacy toward E. coli and S. enterica [714].

MO NPs encompass many elements that have demonstrated powerful antimicrobial properties. CuO NPs synthesized from fungi biomass showed antimicrobial effects against E. coli, S. aureus, Klebsiella pneumoniae, Micrococcus luteus, and B. subtilis [715]. Cu NPs biosynthesized from Aspergillus niger biomass were highly metal resistant and simple to treat [715]. After adsorption of these NPs into the bacterial cell membrane, they disrupt the membrane and cause damage to the bacteria [715]. Another study confirmed the antimicrobial potency of biosynthesized Cu NPs [716]. A medicinal plant, Cissus arnotiana, was used to synthesize Cu NPs and they exhibited promising antibacterial activity against E. coli, with an inhibition zone of 22.20 mm at a concentration of 75 μg/mL [716]. The authors explained this activity through two mechanisms: (1) damaging of the cell membrane and the cellular genetic materials and (2) initiation of oxidative stress [716]. CuO NPs from Camellia sinensis leaf biomass is active against S. aureus (as a gram-positive bacteria) and K. pneumoniae (as a gram-negative bacteria) [717].

ZnO NPs synthesized from biological agents are less toxic, affordable, and ecofriendly compared to traditional chemical and physical synthesis methods [718]. As an antibacterial agent, ZnO NPs from P. granatum fruit peel extract induces oxidative stress that leads to permanent damage to the cell membrane and DNA. Consequently, the ZNO NPs lead to apoptosis of the bacteria. Thus, P. granatum/ZnO-NPs killed both E. coli and Enterococcus faecalis [718]. ZnO NPs from Tabernaemontana divaricata leaf extract exhibited high antibacterial activity against E. coli and S. aureus [719]. Recently, substrates from plants and microorganisms have been used to fabricate magnetic IO NPs that exhibit antimicrobial potency [720]. For example, IO NPs produced from pulp and seed aqueous extract of Citrullus colocynthis, a wild medicinal plant, effectively inhibited the growth of B. subtillis, S. aureus, E. coli, and Pseudomonas aeruginosa pathogenic bacterial strains, and moderately inhibited C. albicans [721]. The iron NPs synthesized from the aqueous extract of Mimosa pudica root, Dodonaea viscosa, A. indica (neem), Kappaphycus alvarezii, and T. procumbens leaf biomass have antibacterial activity [722726]. Moreover, iron NPs from Eucalyptus robusta leaves significantly inhibited S. aureus, P. aeruginosa, and B. subtilis [727]. An inverse relationship between NP size and inhibitory efficacy was observed, which highlights the benefits of iron NPs fabricated from plant aqueous extract [727]. These IO NPs produce ROS, such as hydroxyl radicals, which lead to oxidative stress and bacteria apoptosis [727]. TiO2 is another effective antimicrobial agent in the MO NP group. After activation of TiO2 by the photocatalysis process, it produces ROS, which causes damage to the protein, lipids, mitochondria, and DNA of the bacteria [228]. TiO2 produced from the extract of three rosaceous fruits (plum, peach, and kiwi) peel agriwaste, Artemisia haussknechtii, and Morinda citrifolia leaf biomass exhibited dose-dependent antibacterial activities against E. coli [228,728730]. TiO2 produced from peel agriwaste also inhibited the growth of B. substilis, a gram-positive bacteria, with a zone of inhibition of 17–19 mm at 100 µg/mL concentration [228].

Au NPs have exhibited antimicrobial potency and when these NPs are produced from plant biomass, their solubility becomes better and presents a better antimicrobial effect [731]. According to a recent study, Au NPs synthesized from the fresh leaves of Allium noeanum worked as a strong antibacterial agent against a wide spectrum of bacterium: Streptococcus pneumoniae, B. subtilis, S. aureus, Staphylococcus saprophyticus, Salmonella typhimurium, P. aeruginosa, Shigella flexneri, and E. coli [731]. Also, Au NPs from an aqueous extract of watermelon rind waste was active against E. coli, Bacillus cereus, and Listeria monocytogenes [335]. Another biomass waste used for the biosynthesis of Au NPs was C. maxima peel extract. C. maxima–Au NPs exhibited a strong antibacterial effect against S. aureus and E. coli [333]. In addition, the inhibitory effect slightly increased with the increasing Au NP concentration and, therefore, this biosynthesized Au NP can be used as an effective disinfectant with good antibacterial activity [333].

IQDs, such as CQDs and GQDs, have been used in biomedicine as antimicrobial agents [732]. CDs from the biomass of L. plantarum prevented E. coli biofilm formation, did not interfere with the growth of E. coli and mammalian cells, and had high biocompatibility and low cytotoxicity [733].

5.2 Anticancer activity

Recently, cancer has motivated researchers to seek out more advanced treatments than chemo and radiative therapy. High toxicity and deficient specificity are the major concerns of these traditional therapies [734]. The optimal cancer drug should have a specific targeted delivery system, in addition to appropriate drug-release. Therefore, a variety of nanoscale-based drug carriers have recently been developed and investigated [735]. The typical approach of cancer treatment with NMs is based on the transportation of the chemotherapeutic agent, which has a narrow therapeutic index, reduced cellular penetration, and highly toxic effects [736].

Biomass-based CNMs have shown promise as they have excellent chemical and physical properties, making them excellent nanocarriers with a large efficacy and low systemic toxicity for targeted drug transportation [737].

Biomass-synthesized CNFs have demonstrated anticancer activity based on the drug type. For example, a previous study showed Cu NP dispersed CNFs encapsulated in PVA and cellulose acetate phthalate composite material for drug delivery. The CNFs were capable of lifting the Cu NPs to their surface in the composite, allowing them to control metal ion release into the required cancer sites [738]. Additionally, Wang et al. provided another example of CNF’s anticancer activity through the synthesis of CNF-coated Ni metal, which worked as a drug transporter and favorably delivered the anticancer drug DOX to the targeted cancer cells [739].

Biomass-based CNTs have revealed ecofriendly anti-cancer activity when they were functionalized with chitosan and thereafter coated by DOX to target MDA-MB-231-TXSA breast cancer cells. The CNTs overexpressed CD44, resulting in decreased cell metastasis, inhibition of proliferation, and the beginning of apoptosis. In addition, photothermal therapy has been used for targeting both bladder and prostate cancer [735,736].

G particles originating from C. album and T. procumbens have anti-cancer activity against breast, lung, and colon cancers. The particles produce mitochondrial disruption and DNA damage. Moreover, Lantana camara and T. procumbens precursors of G have shown a cytotoxic effect against A549 cell lines [710,740].

AC originating from biomass materials, such as wood, coal, bamboo, and coconut shells, has shown excellent photothermal properties against human H-1299 lung cancer cells. The AC converts light energy into heat exceeding 42.5°C, which eventually kills cancerous cells [740]. Additionally, AC has shown long-term photothermal therapy as no antibodies or peptides conjugate onto AC particles when they migrate to cancerous cells, thus they are taken up by endocytosis, which consequently prevents NPs from escaping cells once they have penetrated [741].

Inorganic QDs, specifically CQDs, have been proven to possess excellent anti-cancer activity. Interestingly, CQDs from an Andrographis paniculata were applied to both malignant human umbilical vein endothelial cells (HUVECs) and mesothelioma cell lines (H2452). It accumulated in their nucleus or cytoplasm and inhibited their growth in a time and dose-dependent fashion [742]. Furthermore, CQDs originating from Allium fistulosum exhibited high viability against myelogenous leukemia cells (K562, suspension cells) and a breast cancer cell line (MCF-7, adherent cells) through the penetration of cell membranes and distribution over the cytoplasm [742,743]. In addition, CQDs made from Nerium oleander leaf biomass have an anti-proliferative effect in vitro against breast cancer MCF7 cells [742]. Hypocrella bambusae CQDs have shown an efficient capability for the generation of O2 and heat for synergistic photodynamic and photothermal therapy, which exhibits significant anticancer efficacy [744].

Similarly, biomass-synthesized GQDs have shown excellent anti-cancer activity. For example, Ficus racemose-derived GQDs showed excellent photodynamic and photothermal properties, which make them a potent anticancer agent in the targeting of breast cancer cells [744]. Furthermore, a previous study demonstrated that biomass-synthesized GQDs with Cys–berberine hydrochloride (BHC) composite can be used for the delivery of BHC (anti-cancer agent). The GQDs with the Cys–BHC system were also investigated for their antiproliferative activity against HeLa cells and MDA-MB-231 cells [746].

Recent research has also demonstrated the anticancer activity of Au NPs [747]. For example, the anticancer properties of Au NPs synthesized from Anacardium occidentale leaves were studied. These Au NPs showed 23.56% availability on MCF-7 cell lines at a maximum concentration of 100 mg/mL [748]. The apoptosis produced by Curcuma wenyujin–AuNPs was investigated by ROS. The caspases levels in a C. wenyujin–AuNP-treated MDA-MB231/HER2 cell line are shown in Figure 15. Additionally, stable Au NPs made from Taxus baccata extracts have demonstrated potent, selective, dose, and time-dependent anticancer activity on breast (MCF-7), cervical (HeLa), and ovarian (Caov-4) cancer cells [749]. Researchers have used flow cytometry and reverse transcription polymerase chain reaction to conduct in vitro studies, wherein cells were exposed to synthesized Au NPs, and have claimed that the caspase-independent death program was the most viable anti-cancer mechanism of action [749]. The leaf biomass of Mappia foetida was used to efficiently deliver DOX to cancer cells in humans in conjugation with FA [750].

Figure 15 
                  Mechanisms of anticancer activity for Au NPs.
Figure 15

Mechanisms of anticancer activity for Au NPs.

MO NPs have piqued the interest of biomedical researchers due to their structural, physical, and chemical features [751]. The anticancer activity of MO NPs has been demonstrated through binding to cell surfaces or by cellular internalization. Therefore, because of their low stability, some NPs dissociate into their ionic states in body fluid after being administered while other stable NPs directly enter the cancer cells. The formation of ROS by NPs is the main mechanism of action by which cancerous cells are inhibited. [752].

CuO NPs have shown anticancer activity by enhancing the intensity of apoptosis (programmed cell death) in cancer cells [752]. CuO NPs from Ficus religiosa leaf extract instigate anticancer activity in A549 lung cancer through the inhibition of histone deacetylase [753,754]. In addition, CuO NPs reduced the expression of oncogenes while increasing the expression of tumor suppressor proteins in A549 cells [754]. MCF-7 cell viability was reduced by 50% when CuO NPs from C. sinensis leaf biomass were used at a concentration of 50 g/mL. The imaging-based quantification of cellular CuO NP uptake showed a clear dependent toxic activity [717].

In SKOV3 and AMJ13 cancer cells, Cu NPs made from Olea europaea leaf biomass inhibited cell growth and induced apoptosis [755]. CuO/Zn NP hybrids made from Duchesnea indica leaf biomass were used to improve kidney cancer therapy [756].

ZnO NPs have a distinct electrostatic property that aids in the selective targeting of cancer cells. Anionic phospholipids are abundant on the surface of cancer cells, resulting in electrostatic attraction with ZnO NPs. Small ZnO NPs increase the permeation and retention of NPs within tumor cells and thus help the NPs act upon them, while large ZnO NPs promote cellular uptake of ZnO NPs by cancer cells and ultimately leads to cytotoxicity [757]. When compared to normal cells, ZnO NPs produce a large amount of ROS in cancer cells, resulting in a large amount of oxidative stress from which the cancer cells die [758]. Furthermore, the synthesis of ZnO NPs from Laurusobilis leaves has shown anticancer activity in A549 lung cancer. Normal murine macrophage RAW264.7 cells were found to be unaffected by ZnO NPs, but the NPs were effective in inhibiting the viability of human A549 lung cancer cells at greater concentrations of 80 g/mL [759]. Additionally, the ZnO NPs synthesised from Ecliptaprostrata leaves have been tested on the human liver carcinoma line (HeO-G2) [760] while ZnO NPs synthesised from Ziziphus nummularia leaves have shown anticancer activity against the HeLa cancer cell line [761].

Primary solid–solution NPs, or ions, have potential applications in drug and gene delivery, in specific medical specialties and as theranostic NPs [754]. In essence, two distinct approaches for treating tumors with SPIONs are frequently used. Magnetically evoked hyperthermia, drug targeting, and selective neoplasm growth suppression are implemented. Researchers have shown that cancer cells become more aggressive when exposed to iron compound NPs. Consequently, it was concluded that these NPs could be used to treat tumors safely, without harming healthy cells. In addition, researchers have observed how much ROS was produced when A549 cancer cells were treated with ions, which accordingly induced autophagy [754]. SPIONs successfully synthesized from fruit peel biomass had anticancer activity against HeLa [762] and iron NPs synthesized from brown seaweed biomass had anti-cancer activity [763].

TiO2 NPs from Vigna radiata legume extract effectively killed HeLa cells through photocatalysis, which suggests that TiO2 NPs could be used to decrease the recurrence of osteosarcoma and chondrosarcoma by inducing cytotoxicity in bone tumor cells [764,765]. This can be achieved by increasing ROS levels. Interestingly, these findings suggested that TiO2 NPs could be used to reduce or prevent osteosarcoma and chondrosarcoma recurrence [764]. Table 15 shows the anticancer activity of recycled NPs.

Table 15

Application of recycled NPs as therapeutic anti-cancer agents

NM Biomass sources Applications Ref.
GNPs Chenopodium album Anti-cancer activity against breast, lung, and colon cancers [710]
GNPs Tridax procumbens Anti-cancer activity against breast, lung, and colon cancers [766]
GNPs Lantana camara leaves Cytotoxic effect against A549 cell lines [711]
AC Wood biomass Anti-cancer activity against human H-1299 lung cancer cells [741]
AC Coal biomass Anti-cancer activity against human H-1299 lung cancer cells [741]
AC Bamboo biomass Anti-cancer activity against human H-1299 lung cancer cells [741]
AC Coconut biomass Anti-cancer activity against human H-1299 lung cancer cells [741]
CQDs Andrographis paniculata Anti-cancer activity against malignant HUVECs and mesothelioma cell lines (H2452) [742]
CQDs Allium fistulosum Anti-cancer activity against myelogenous leukemia cells (K562, suspension cells) and breast cancer cell line (MCF-7) [743]
CQDs Nerium oleander leaves Anti-cancer activity against breast cancer MCF7 cells [743]
CQDs Hypocrella bambusae trees Anti-cancer activity [744]
GQDs Ficus racemose leaves Anti-cancer activity against breast cancer cell [745]
Au NPs Anacardium occidentale leaves Anti-cancer activity against human cell lines for breast cancer (MCF-7 cell lines) [748]
Au NPs Taxus baccata extract Anti-cancer activity against human cell lines for breast (MCF-7), cervical (HeLa), and ovarian (Caov-4) cancer cells [749]
Au NPs Mappia foetida leaf Deliver DOX to cancer cells [750]
Toxic to many human cancer cells, such as HeLa, SiHa, MDA-MB-231, and Hep-G2 [750]
CuO NPs Ficus religiosa leaves Anti-cancer activity against A549 lung cancer [757,759]
CuO NPs Camellia sinensis leaves Anti-cancer activity against MCF-7 (breast cancer cells) [717]
CuO/Zn NPs Duchesnea indica leaves Improve kidney cancer therapy [756]
ZnO NPs Laurus nobilis leaves Anti-cancer activity against A549 lung cancer [759]
ZnO NPs Ecliptaprostrata leaves Anti-cancer activity against human liver carcinoma line (HeO-G2) [760]
ZnO NPs Ziziphus nummularia leaves Anti-cancer activity against human cervical epithelial cancer cells (HeLa) [761]
SPIONs Fruit peel biomass Anti-cancer activity against human cervical epithelial cancer cells (HeLa) [762]
Iron NPs Brown seaweed biomass Anti-cancer activity against human cell lines for breast cancer, leukemia, liver cancer, and cervical cancer [763]
TiO2 NPs Vigna radiata legume Anti-cancer activity against Mg 63 osteosarcoma and chondrosarcoma cancer cell lines [764,765]

5.3 Antioxidant activity

An antioxidant is a material that prevents molecules within a cell from oxidizing. During the biological oxidation reaction, free radicals are produced, and a chain reaction is started concurrently because the radicals are reactive. A cell may be damaged or may die as a result of this [767]. Antioxidants bind to free radicals, stopping harmful chain reactions and converting them to harmless byproducts. Antioxidants thus reduce oxidative stress and are important in the treatment of diseases caused by free radicals, such as heart disease, neurodegenerative disorders, cancer, and the aging process.

However, the efficiency of natural and synthetic antioxidants is limited due to poor absorption, difficulty crossing cell membranes, and degradation during delivery, all of which contribute to their low bioavailability [768]. Antioxidants have been covalently connected to NPs to provide improved stability, sustained release, compatibility, and targeted delivery of antioxidants [768]. Therefore, we now discuss some examples of NPs used as antioxidants and their biomass waste-derived origins, as shown in Table 16.

Table 16

Application of recycled NPs as antioxidants

NM Biomass sources Ref.
CQDs Green tea waste [769]
Au NPs Allium noeanum leaves [731]
Au NPs Abroma augusta L. bark [770]
Au NPs Watermelon rind [335]
ZnO NPs Punica granatum peel [718]
Iron NPs Camellia sinensis (green tea) leaves [772]
Iron NPs Murraya koenigii leaves [773]
Iron NPs Phoenix dactylifera [771]
TiO2 NPs Kola seed [774]
TiO2 NPs Artemisia haussknechtii [730]
TiO2 NPs Psidium guajava [233]
TiO2 NPs Morinda citrifolia leaves [728]

CQDs were made using a carbonization technique that used waste green tea leaves as a carbon source. 2,2-diphenyl-1-picrylhydrazyl (DPPH) quenching by hydrogen atom transfer from the carboxyl, hydroxyl, and/or amino groups for CQDs is a potential mechanism for DPPH reduction by CQDs [769]. Au NPs created as a waste product from an aqueous extract of A. noeanum leaves, Abroma augusta L. bark, or watermelon rind have exhibited antioxidant properties [335,731,770]. This may be due to the ability of Au NPs to neutralize and scavenge DPPH free radicals by donating hydrogen ions or electrons [335,731,770]. The antioxidant activity of iron NPs synthesized from Phoenix dactylifera, which contain a high amount of polyphenols, has been well established. Their antioxidant potential was carried out by determining the products from oxidation or by assessing the ability to retain the radicals of the reaction patterns [771]. Antioxidant properties have also been demonstrated in iron NPs derived from C. sinensis (green tea) and Murraya koenigii leaves [772,773].

After incubation, biosynthesized TiO2 NPs were capable of causing DPPH decolorization, indicating that they are antioxidants in nature. DPPH was scavenged in a dose-dependent manner at tested concentrations of 10–80 g/mL, yielding responses of 32.61–62.06% [772,773]. Kola seed-mediated particles have been the most intense among photosynthesized TiO2 NPs, with the least activities obtained for KS–TiO2 NPs, which had the highest performance of 52.37% [774]. Antioxidant activities have been also reported for TiO2 NPs made from fruit peel agriwaste, L. siceraria, P. dulce, P. guajava, Allium eriophyllum, A. haussknechtii, and the leaf biomass of M. citrifolia [228,233,728,730]. Furthermore, plant aqueous extract and synthesized TiO2 NPs were found to possess maximum antioxidant activity compared to ascorbic acid [233].

5.4 Nanodrugs and nanovaccines

Nanopharmaceuticals combine nanotechnology with biomedical and pharmaceutical sciences. Nanomedicine is a new and rapidly growing field. NPs can be used in drug formulations due to their pharmacokinetics, safety, efficacy, and targeting ability [775]. Many drug-based NPs have enrolled in clinical trials, however, drug-based NPs face a lot of challenges because of their toxicity issues, need for better characterization, and the absence of regulatory guidelines [775].

IO NPs have been used in many drugs as iron replacement therapy. These include Ferrlecit (sodium ferric gluconate complex in sucrose injection, Sanofi-Aventis, US), Venofer (iron sucrose injection, American Regent, Inc.), Dexferrum (iron dextran injection, American Regent, Inc.), and Infed (iron dextran injection, Actavis Pharma), which are all used in the treatment of anemia associated with chronic kidney disease [775,776]. These nano-formulations contain an iron oxide core covered with hydrophilic polymers, such as dextran or sucrose that allow the iron to be dissolved slowly after injection. These formulations permit fast administration of large doses without increased iron-free blood levels, preventing toxicity [777]. SPIONs are biodegradable, have low toxicity, and remain in blood circulation for a long time. SPIONs made from fruit peel biomass respond strongly when exposed to magnetic fields, releasing energy that can be used in targeting specific tumors [762]. Nanotherm, for example, is a drug that treats glioblastoma tumors. A different magnetic field is applied to selectively heat particles after injection of Nanotherm directly into the tumor [778]. This leads to local heating of the tumor to 40–45°C, resulting in programmed and non-programmed cell death. Nanotherm is now awaiting Food and Drug Administration (FDA) approval.

The negative nature of functional groups loaded on CNFs made from chitin biowaste has enabled their electrostatic binding to the protonated drug R-NH3+, as in the DOX anticancer drug [779]. In the last decade, CNTs made from agricultural biomass sources have received more interest in research applications in the field of drug delivery [34]. Various strategies for binding different CNT drugs were established through either covalent binding or non-covalent adsorption [780]. Functionalization of CNTs is therefore required for benign compatibility and good solubility. Additionally, GO has the benefits of low cost, two external surfaces, simple manufacturing, and alteration, and lack of toxic metal particles. GO also has an ultrahigh surface area for effective drug binding for all sp2 carbon atoms exposed on its surface. In addition, planar GO sheets for future multi-modal imaging and treatment applications can easily be complexed with functional NPs [780]. G made from biomass is also gaining popularity in research applications in the field of drug delivery [781,782].

Due to the large surface area of Au NPs, they are useful in the delivery of drugs. Drug molecules can bind to the conjugate Au NPs by physical absorption or by a covalent or ionic bond. DOX is an anticancer drug that can attach to Au NPs via a pH-sensitive linker. This DOX–Au NP attachment allows the intracellular release of DOX from Au NPs inside acidic organelles. This release allows a rapid increase in the concentration of intracellular DOX, enhancing therapeutic efficacy in tumor cells [783]. M. foetida leaf biomass and onion peel extract were used as a bioreductant in the synthesis of Au NPs, which were then used to efficiently deliver DOX to cancer cells [750,784].

The presence of efficient fluorescent labels makes QDs suitable for drug delivery systems as these labels track the metabolism process of the drug in the body. QDs are also able to cross cell membranes and their large surface area provides several drug targeting attachment sites. GQDs can load drugs on their surface hydrophobically or through noncovalent π–π interactions [785]. GQDs are also biocompatible and the small size of CQDs make them ideal for drug delivery. CQDs made from crab shell have enabled specific targeting to cancer cells [517] while those made from bamboo-leaf cellulose have been used to deliver DOX to cancer cells [786]. Sugarcane bagasse CQDs have exhibited a greater drug loading capacity [787].

In summary, NPs have several characteristics that are useful in drug manufacturing. Their biocompatibility and small size makes them useful for the delivery of drugs and carrying the drug into the cell while their fluorescence or photoluminescence can be used to track the metabolism of the drugs in vivo. Additionally, the magnetic and thermal energy of NPs kills tumor cells when exposed to light or a magnetic field.

Nanotechnology has merged with vaccine development in the fight against diseases caused by bacterial or viral infections, as well as malignant tumors, resulting in nanovaccines, which are crucial [788]. Nanovaccines have many advantages over conventional vaccines as antigens can be encapsulated in nanocarriers to avoid antigenic degradation. Also, antigen-presenting cells (APCs) can quickly process and phagocytize nanovaccines [789].

NMs have provided one-of-a-kind opportunities to increase the therapeutic efficacy of cancer vaccines’ antigens while molecular or nanoadjuvants, and nanocarriers are commonly used in nanovaccines [790]. In melanoma, colon cancer, and human papillomavirus E6/E7, nanovaccines have triggered significant immune responses that inhibited tumor growth [791]. Tumor-specific immune responses can be induced by cancer vaccines and T cells that are specific to tumors and ensure that they are activated and expanded. Recent progress in NP-based nanovaccines has focused on the co-delivery of tumor-specific antigens and adjuvants to APCs, such as dendritic cells (DCs) [789].

Immunization with colloidal gold conjugated to haptens (small molecules that can only induce an immune response when attached to a carrier) and antigens resulted in higher antibody levels than immunization with complete Freund’s adjuvant. Furthermore, when compared to complete Freund’s adjuvant immunization, the amount of antigen required with colloidal gold is lower [792]. In addition, Au NPs are appealing nanocarriers because they are non-toxic, inert, and easily endocytosed by DCs. DCs can filter vaccine peptides on the particles to activate cytotoxic T lymphocytes (CTLs) and uptake Au nanovaccines with minimal toxicity. Au nanovaccines with high peptide density stimulate CTLs better than free peptides and have a lot of potential as vaccine carriers [793].

SPIONs are the NPs used for vaccine delivery [794]. SPIONs provide a novel way to activate the humoral and cellular immune systems in the fight against cancer. SPIONs coated with recombinant heat shock protein 70 (Hsp70), which is known to chaperone antigenic peptides, had increased immunostimulatory ability. Hsp70–SPIONs bind to tumor lysates and deliver immunogenic peptides to DCs, triggering a tumor-specific CD8+ cytotoxic T cell response [795]. The use of DCs pulsed with Hsp70–SPIONs and tumor lysates to immunize C6 glioma-bearing rats resulted in a delay in tumor development (as measured by MRI) and an improvement in overall survival. Parallel to this, increased interferon secretion was found in the serum of these animals and immunohistological examination of subsequent glioma cryosections showed increased infiltration of memory CD45RO+ and cytotoxic CD8+ T cells. The results demonstrate that magnetic nanocarriers, such as SPIONs coated with Hsp70, can be used as a medium for enhancing anti-cancer immune responses [795]. Many basic objectives in this field include magnetic properties of IO NPs, complete control over particle size distribution, ability to carry different types of biomolecules with respect to surface functional groups, low-cost development, and good immune status [794].

DC vaccines have a lot of promise in cancer immunotherapy but their anti-tumor effectiveness is hampered by their poor design and the immunosuppressive tumor microenvironment. Semiconductor QDs have been designed to serve as fluorescence nanoprobes, immunomodulatory adjuvants, and nanocarriers for tumor antigens and Toll-like receptor 9 agonists, among other applications [796]. QD-pulsed DC vaccines allow for spatiotemporal lymphatic drainage monitoring and DC immunotherapy efficacy evaluation, as well as potent immune activation. Designer DC vaccines combined with macrophage polarization elicits a powerful immune response that stimulates both innate and adaptive antitumor immunity while improving the immunosuppressive tumor microenvironment. As a unique combination treatment, this approach significantly increases antigen-specific T-cell immunity, inhibiting local tumor growth and metastasis in vivo. This research could lead to a new cancer immunotherapy treatment [797]. Table 17 shows the application of recycled NPs in nanodrugs and nanovaccines.

Table 17

Application of recycled NPs as nanodrugs and nanovaccines

NM Biomass source Applications Ref.
Au NPs Mappia foetida leaf biomass DOX delivery to cancer cells [750]
Au NPs Onion peel extract Targeted drug delivery for treatment of cancer [784]
Au NPs M. foetida leaves Nanovaccine [750]
Ag/Au Parkia roxburghii Nanovaccine [306]
CQDs Sugarcane bagasse Provides the NM with greater drug loading capacity [787]
CQDs Crab shell Enables specific targeting to cancer cells [517]
CQDs Bamboo-leaf cellulose DOX delivery to cancer cells [786]
CQDs Nerium oleander leaf Nanovaccine [743]
SPIONs Fruit peel biomass Drug delivery [762]
Iron oxide Fruit peel biomass Nanovaccine [762]
G/GO NPs Biomass-synthesized G Drug delivery [782]
CNTs NPs Agricultural biomass sources Drug delivery [34]
CNFs NPs Chitin biowaste Drug delivery [779]
CNMs Plastic bags Nanovaccine [797]

6 Cytotoxicity of NMs

6.1 CNMs

The CNMs’ complexity and variety in size, chemical compositions, shape, charge, manufacturing methods, and surface functionalization are all important variables in their cytotoxicity [798]. CNMs can enter the body by a variety of methods including inhalation, oral administration, and injection. They can easily move throughout organs to the circulatory system [799]. When CNMs are injected intravenously or taken orally, they might cause inflammation in vulnerable organs such as the liver, kidneys, and lungs [800].

The cytotoxicity of CNTs in healthy tissues is a serious challenge in biomedical applications. As a result of the various techniques of synthesis, CNTs vary in size, shape, structure, and purity [801]. CNTs cytotoxicity is related to their synthesis process, length, functional group(s), structure, surface-to-volume ratio, concentration, composition, amount of oxidation, and the extent of aggregation [802].

Furthermore, insufficient removal of metal catalysts utilized during CNTs preparation has been linked to their increased cytotoxicity [803]. The CNTs’ limited biocompatibility, on the other hand, is a major barrier to their usage in biomedical applications due to their poor solubility. The hydrophobic surface of CNTs as well as their tendency to aggregate are thought to be contributing factors in their toxicity in vitro [804]. However, by coating the surface of CNTs with biocompatible surfactants or polymers, these adverse effects can be reduced [805]. Oxidative stress, cell membrane injury, DNA damage, and death are all potential pathways for CNTs cytotoxicity [806].

Structure, surface chemistry, number of layers, functional groups, and the employment of reducing agents for functionalization, all play a role in G and its derivatives’ cytotoxicity [807]. The principle mechanism of cytotoxicity of G-based NMs is the generation of ROS [808].

Normal cells may be harmed by G-based NMs, because they disrupt the physiological conditions. When G-based NMs are used, a lot of ROS is produced. Increased levels of ROS can cause diseases such as diabetes [809], Alzheimer’s disease [810], atherosclerosis [811], and carcinogenesis [812]. Polysaccharide modification of G NMs is a promising method for lowering their toxicity and improving their targeting ability, which improves biotherapeutic efficacy [813].

6.2 IQDs

In 2011, the US FDA approved the first human clinical trial of QD technology. Most chemotherapeutics and cytotoxic medicines are now given as QDs for an improved pharmacological action [814]. The major concern for the use of QDs in biomedical application is their toxicity. QDs toxicity is determined by their size, dose, delivery method, and the capping material [814]. Although the regulatory status of QDs is unclear, they are nevertheless considered safe to use. However, the development of harmless QDs such as CQDs and GQDs could help to overcome this to some extent [814].

The main way of reducing the toxicity of QDs is using metal-free materials for QDs preparation [815]. In addition, biocompatible functionalization was also used to reduce the toxicity of QDs. QDs can be enclosed in phospholipid micelles for biological applications, resulting in no surface modifications and the retention of optical properties [816]. The other approach is antibody conjugation [814].

6.3 MO-based NMs

MOs are likely to accumulate in the environment after their use, generating adverse effects on the environment and human health, due to their higher chemical reactivity resulting in an increased generation of ROS [817]. Indeed, the surface of MOs is a major factor in their toxicity as a result of the interaction of their surfaces with the biological system [818]. Different MOs can be found in nature, however, some of them have a wide range of biomedical applications, including IO NPs, TiO2 NPs, ZnO NPs, and CuO NPs [819].

The cytotoxicity of IO NPs is one of the major challenges to their translation into biomedical applications. Generation of ROS, including hydroxyl radicals, superoxide anion, and nonradical H2O2, is responsible for the majority of IO NPs intracellular cytotoxicity [820]. The generation of ROS from the NP surface, ROS creation by leaching of iron molecules, modifying mitochondrial functions, and stimulation of signaling pathways are the four primary sources of oxidative damage in response to IO NPs [821]. Surface coating is one method for making IO NPs non-toxic and biocompatible [822].

With rapid nanotechnology development, TiO2 NPs and ZnO NPs are widely used in various fields. People working in such environments, as well as researchers in laboratories, are more likely to be exposed to TiO2 NPs and ZnO NPs [823,824]. Furthermore, increasing data suggest that TiO2 NPs concentrations are elevated in animal organs following systematic exposure, and that these accumulated NPs may cause organ damage. Oxidative stress, autophagy, apoptosis, inflammatory response, genotoxic effects, and signaling pathways all contribute to TiO2 NPs toxicity [823]. Cell membrane damage, cytotoxicity, and increased oxidative stress have been described in diverse mammalian cell lines as the most common harmful effect of ZnO NPs [825]. ZnO NPs have been shown to have genotoxic potential in both in vivo and in vitro experiments, in addition to cytotoxicity [826].

CuO NPs have been shown to cause harmful effects on the liver and kidneys in many experiments [827]. In experimental animals, CuO NPs have caused severe damage in the liver, spleen, and kidneys. Highly reactive ionic copper is generated after oral administration and interaction with gastric fluid, which is then deposited in the kidneys of exposed animals [828].

6.4 Au NPs

Au NPs have received a lot of interest in the biomedicine field because of its electrical, chemical, thermal, mechanical, and optical properties, With the high potentials, the high risk of toxicity came, as a result of their interaction with biological tissues and biomolecules [829]. In vivo and in vitro experiments on Au NPs were carried out. Both showed some oxidative damage to organs and cell lines in vivo and in vitro respectively, with the liver, kidney, and spleen being the most impacted [829].

The size and shape of Au NPs are the most essential factors that contribute to their cytotoxicity, because they are directly associated to the process of cellular internalization [830]. The cytotoxicity of Au NPs is size dependent, with smaller (1.4 nm) Au NPs being more cytotoxic than larger (15 nm) ones [831]. In HeLa cells, SK-Mel-28 melanoma cells, L929 animal fibroblasts, and mouse monocytic/macrophage cells, Pan et al. found that 1.4 nm Au NPs caused rapid cell death through necrosis, whereas 1.2 nm Au NPs caused cell death through apoptosis [831]. The large surface areas of these extremely small particles can contribute to the production of ROS. ROS injure cells by destroying proteins, membranes, DNA, and other organelles like the mitochondria, cytoplasm, and nucleus [829].

Vales et al. found that, in addition to size and shape, surface functionalization of Au NPs has a role in their cytotoxicity. Three functionalization were used in this study: negative (carboxylate), positive (ammonium), and neutral (PEG). In comparison to anionic and neutral Au NPs, cationic Au NPs were more cytotoxic. A positive surface charge appears to exacerbate the cytotoxicity of Au NPs [832].

7 Conclusion and future prospects

To summarize, the authors have shed light on valuable NMs that can be extracted from waste sources originating from everyday life, including biomass wastes, cooking oil, and industrial wastes, to achieve “waste-to-wealth” and meet the “zero-waste” challenge. Different CNMs, including inorganic QDs, various MOs, and Au NPs, can be easily extracted from the above-mentioned sources. Then the different synthesis approaches used to synthesize these NMs, which could be classified into top-down and bottom-up routes, were presented. Additionally, their potential roles in the early detection of serious diseases, with a special focus on their roles in fluorescent imaging, magnetic imaging, and when acting as biosensors, were summarized. Moreover, the promising therapeutic modalities of NMs as antimicrobial, anticancer, antioxidant agents, and as nanodrugs and vaccines were analyzed in detail.

Many other recyclable NMs are valuable for biomedical applications. Recently, palladium and platinum NPs were introduced as potential and novel mineral derived NPs synthesized from different sources of waste via diverse green synthesis strategies [833837]. They are amongst the widely used NPs for applications in biomedicine like drug delivery, biosensors, imaging, photothermal therapy, cosmetics, antimicrobials, and therapeutics for many afflictions (AIDS, cancer, and malaria), and implants [838842]. Furthermore, they have unique anticancer [843], antioxidant, and antibacterial capabilities [844]. However, further research is needed to highlight their role in the early detection of different diseases. Although RNMs have shown many outstanding characteristics such as cost-effectiveness, ease of manipulation, and good physiological properties, many investigations are still required for their further isolation and purification. In addition, the use of RNMs for other biomedical applications, such as bio-scaffolds in tissue engineering and regenerative medicine and wound-healing applications, has not yet been addressed.


These authors contributed equally to this work.


Acknowlegement

A. Matsuda and G. Kawamura acknowledge Japan Society for Promotion of Science (JSPS) KAKENHI Grant No. 18H03841 and No. 21K18823, for partially funding this study.

  1. Funding information: Japan Society for Promotion of Science (JSPS) KAKENHI Grant No. 18H03841 and No. 21K18823.

  2. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Conflict of interest: The authors state no conflict of interest.

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Received: 2021-08-16
Revised: 2021-09-26
Accepted: 2021-09-27
Published Online: 2021-10-22

© 2021 Mohamed Abd Elkodous et al., published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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