Elsevier

Journal of Cleaner Production

Volume 241, 20 December 2019, 118189
Journal of Cleaner Production

Melamine grafted chitosan-montmorillonite nanocomposite for ferric ions adsorption: Central composite design optimization study

https://doi.org/10.1016/j.jclepro.2019.118189Get rights and content

Highlights

  • A novel nanocomposite adsorbent synthesized based on chitosan, Nano-Montmorillonite, and melamine.

  • Use of the synthesized nanocomposite as a novel effective adsorbent for the ferric ions removal from aqueous solution.

  • CCD of RSM has been employed for the optimization of the removal of ferric ions using the synthesized nanocomposite.

  • The adsorption equilibrium, kinetics and thermodynamics have been studied.

Abstract

Chitosan-based nanocomposites are considered to be promising candidates to for application in water treatment technology due to their distinguished physicochemical properties. In the present work, a new melamine grafted chitosan nanocomposite has been synthesized as an effective material for ferric ions adsorption. The nanocomposite has been synthesized via graft polymerization of chitosan using glutaraldehyde/epichlorohydrin crosslinkers in the presence of 0.1% of Nano-Montmorillonite (w/w % based on chitosan). Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), thermal gravimetric analysis (TGA), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques have been utilized for the characterization of the synthesized nanocomposite. Central composite design (CCD) of response surface methodology (RSM) has been applied for determination of the optimum conditions for the adsorption of ferric ions. Under the optimum conditions, the nanocomposite shows 99.97% for ferric ions removal percent with good reusability till third cycle. Kinetic, isothermal, and thermodynamic analyses have been studied to have deep insights into the mechanism of ferric ions adsorption on the synthesized nanocomposite.

Introduction

Heavy metal pollution is considered to be an increasingly serious environmental problem in recent decades, causing various disorders and diseases (Ma et al., 2018a,b). These metal ions are commonly existing in waste streams from mining process, metal plating, electronic devices, dyeing, petroleum refining, and tanneries (Alizadeh et al., 2018). Heavy metal ions are highly toxic, non-biodegradable and can accumulate in the environment causing serious pollution in surface and groundwater. Therefore, accumulation of heavy metal ions in the living bodies through food chain even at very low concentration can cause severe diseases, such as dementia, itai-itai disease, leukemia, cancer, etc (An et al., 2018). Among them, iron whose high concentrations in industrial and ground water are toxic and may cause human health and environmental problems (Demlie et al., 2014). Severe iron poisoning can damage the gastrointestinal tract and liver due to free radical production through lipid peroxidation (Deugnier and Turlin, 2007). On the other hand, iron is a vital element due to its application in manufacturing industries, namely, steel, aeronautic, car, and coating industries (Parambadath et al., 2015). Therefore, developing new technologies and materials for adsorption of Fe3+ is of special interest for the scientific community.

In the last few decades, some processes, including ion exchange (Vaaramaa and Lehto, 2003), solvent extraction (Andersen and Bruno, 2003), bioremediation (Berbenni et al., 2000), limestone treatment (Aziz et al., 2004), oxidation, chlorination, and ozonation followed by filtration (Ellis et al., 2000) have been used for iron removal from aqueous solution. On the other hand, most of these methods have several limitations, such as low efficiency especially when it comes to low ion concentrations (<100 mg L−1), and secondary pollution (Sharma and Tiwari, 2016; Bouzit et al., 2018; Meng et al., 2018). Among them, adsorption is the most powerful technique because of its simple design, manageable operation, the possibility of metal recovery, high efficiency of heavy metal removal from diluted solutions, and regeneration of the adsorbent (Habiba et al., 2017). Consequently, the selection of appropriate materials for the adsorption of metal ions at trace levels from aqueous solutions is crucial for developing an applicable method. For example, carbon-based adsorbents (Jin et al., 2018), phosphatidylcholine (Wang et al., 2016), aluminum silicotitante (Borai et al., 2018), natural apatite (Qian et al., 2014), alginate–mangrove composite beads coated by chitosan (Jawad et al., 2016), macroporous glass (Kuznetsova et al., 2018), and graphene oxide (Konicki et al., 2017) have been employed for the removal of Fe3+.

Recently, the advancement in nanotechnology suggested the promising future of nanomaterials for water treatment in an economical manner along with efficient adsorption capacities for heavy metal ions (Alqadami et al., 2017). Polymer-based nanocomposites, which combine advantages of both polymers and nanoparticles, have paid increasing attention because of their excellent biocompatibility, biodegradability and non-toxicity (Zhao et al., 2011). Recently, chitosan (CS) nanocomposites become materials of choice due to its ease of functionalization and absence of internal diffusion, chemical accessibility, and attractive surface area. Hence, CS nanocomposites have been used as sorbents for heavy metals removal from aqueous solution (Olivera et al., 2016; Nasiri et al., 2018). It is known that functionalization of CS with Nano-Montmorillonite improves functional, barrier, mechanical, and thermal properties of the biopolymer-based composites while maintaining their biodegradability. Montmorillonite (MMT) is considered to be one of the most abundant clay minerals having 2D sheet-like morphology. The MMT sheets consist of three layer structural units, which are composed of two SiO4 tetrahedral sheets and a central AlO4(OH)2 octahedral sheet. Substitutions within the lattice structure of Al3+ for Si4+ in the tetrahedral sheet and of ions of lower valence, particularly Mg2+, for Al3+ in the octahedral sheet result in a net negative charge on the clay surfaces. The charge imbalance is offset by the exchangeable cations such as Ca2+ or Na+ in the interlayer. Thus, MMT has the capability to adsorb cations via ion-exchange mechanism. In recent, MMT has attracted increasing attention as relatively cheap adsorbent owing to its distinguished properties of high surface area as well as ion-exchange ability (Tong et al., 2018). On the other hand, the combination of both synthetic and natural polymers leads to new materials having unique properties. The most efficient and common method of modifying functional and structural properties of natural polymers is chemical grafting. Graft copolymerization of natural polysaccharides becomes a significant resource for developing advanced materials since it can enhance the functional properties of natural polymers. The grafting leads to combining the properties of both polymers due to the attachment of synthetic polymeric chains on backbone of natural polysaccharides (Iftekhar et al., 2018). One of these synthetic polymers is melamine (Mel). Mel has a number of amino groups, indicating its great potential for the heavy metal ions removal (Yin et al., 2018). Thus, the introduction of Mel into chitosan montmorillonite composite is very meaningful.

Statistically designed experiments that investigate Fe3+ adsorption treatment systems have been conducted in a limited literature (Savic et al., 2012; Cerrahoğlu et al., 2017).

To the best of our knowledge, there has been no study conducted until now for the synthesis of melamine grafted chitosan montmorillonite nanocomposite and use it as an adsorbent for Fe3+ removal applying response surface methodology (RSM) modeling. Central composite design (CCD) is the most popular RSM approach. The RSM-CCD application possesses some advantages, such as experimental accuracy, minimization of experimental trials, and the amount of information gained for measuring goodness of fit (Khalid et al., 2019). Thus, RSM based on CCD has been applied for the identification and optimization of the Fe3+ ions adsorption by the synthesized nanocomposite. Studied experimental variables are the initial pH, amount of adsorbent, initial metal ion concentration, and temperature. All the variables are simultaneously used in order to determine their relative effects.

Section snippets

Materials and chemicals

Chitosan (MW. = 100 kDa) with degree of deacetylation 93%, Nano-montmorillonite, gluteraldhyde 25%, epichlorohydrin, melamine, ferric chloride 97%, and chromium(III) chloride hexahydrate 96% were delivered from Sigma-Aldrich. Otherwise specified chemicals were of reagent grade and utilized without further purification. Doubly distilled water was used throughout the experiments.

Instrumentation

The prepared nanocomposite was characterized with different techniques. FTIR were obtained using a Nicolet Nexus

Characterization of the adsorbents

Fig. 1a shows the FTIR spectra of CS, Nano-MMT, CS/MMT, and CS/MMT/Mel sorbent before and after the Fe3+ sorption.

CS has characteristic peaks for C–H stretching around 2924 and 2860 cm−1 due to the stretching vibrations in addition to a broad intense peak at approximately 3400 cm−1 correspond to OH and NH stretching. The absorption around 1650 cm−1 is attributed to the stretching vibrations of Cdouble bondO, amide group as well as the deformations vibrations of OH and NH. Other absorption is seen at

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