Elsevier

Polymer

Volume 132, 6 December 2017, Pages 368-393
Polymer

Feature article
Recent developments on nanocellulose reinforced polymer nanocomposites: A review

https://doi.org/10.1016/j.polymer.2017.09.043Get rights and content

Highlights

  • Various processing techniques of nanocellulose composites are studied.

  • Comparison of CNC- and CNF-reinforced nanocomposites are investigated.

  • Recent development of cellulose nanocomposites is presented.

Abstract

The development of nanocellulose and nanocellulose-based composites and materials has attracted significant interest in recent decades because they show unique and potentially useful features, including abundance, renewability, high strength and stiffness, eco-friendliness, and low weight. This review addresses critical factors in the manufacturing of nanocellulose composites, followed by introducing and comprehensively discussing various nanocellulose composite processing techniques. The review also provides advances on rubber and thermoset polymer matrices, such as unsaturated polyester resin, formaldehyde resins, and polyethylene terephthalate, used to reinforce cellulose nanocrystals (CNCs) or cellulose nanofibers (CNFs). The paper concludes with new findings and cutting-edge studies on electrospun nanocellulose composites. Different aspects, including preparation methods, morphology, mechanical behavior, thermal properties, and barrier action, as well as comparisons of CNC- and CNF-reinforced rubbers or thermoset polymers and electrospun composites, are investigated.

Introduction

Presently, renewable and biodegradable materials are receiving extensive attention from both scientific and industrial communities, because the use of conventional petroleum-based polymer products has created ecological threats such as global warming and plastic pollution. Cellulose is the most abundant natural polymer, and has been used to propose rational solutions for these issues. In recent decades, the interest in nanostructured celluloses, or nanocellulose, has sharply increased because of the specific chemical and physical properties of these materials. Nanocelluloses are typically distinguished into two main groups: i) those obtained by acid treatment, referred to as cellulose nanocrystals (CNCs), and ii) those produced mainly by mechanical disintegration, called cellulose nanofibers (CNFs). The final chemical and physical properties of nanocellulose depend directly on the source and preparation conditions of the cellulose. According to their different properties, CNCs and CNFs are used for different applications.

The use of nanocellulose as reinforcement in nanocomposites has become a popular research topic. In addition to the numerous advantages of nanocellulose, such as low cost, low density, renewability, low energy consumption, high specific properties, biodegradability, and relatively good surface reactivity, it shows better properties as a reinforcing phase in nanocomposites as compared to micro- or macro-cellulose composites. The tailorability, design flexibility, and processability of nanocellulose–polymer composites permit extensive utilization in the automotive, packaging, electronics, and biotechnology industries, among others. However, some disadvantages are associated with nanocellulose use as reinforcing material, particularly its high moisture absorption, poor wettability, incompatibility with most polymeric matrices, and limitations in processing temperature. These drawbacks have encouraged scientists to focus on these issues; various methods, by the modification of nanocellulose or polymer matrices or by all-new processing techniques, have been proposed to produce high-performance nanocellulose-reinforced composites with good properties.

Although many publications have reported on the use of nanocellulose-reinforced polymer composites, few review papers have discussed this topic [1], [2], [3], [4], [5], [6], [7], [8], [9]. Certain recent advances and findings have not been addressed satisfactorily in previous publications. Most prior publications focused on the use of either CNC or CNF, while here, we provide a comparative study on the effects of CNC versus CNF on the properties of composites incorporating them.

The purpose of this review is to combine all recent research to provide readers with a comprehensive overview of the advanced science and engineering of nanostructured cellulose composites. It provides an in-depth look at nanocellulose types of CNC and CNF, composite processing, and the effects of nanocellulose on the mechanical, thermal, crystalline, barrier and other properties of matrix materials, including rubber and thermoset polymers such as epoxy and unsaturated polyester. Following this review, we extensively discuss electrospun nanocellulose composites, their preparation, and their properties.

Section snippets

Nanocellulose composite processing

Nanocellulose particles and related materials can be prepared by different processing techniques that directly influence the final material properties. Particle organization, degradation, and interaction with the matrix are some examples discussed further in this section.

First, it is important to emphasize that, independent of the selected processing method, the major challenge in nanocomposite preparation is the quality of particle dispersion. Despite relevant advances in recent decades,

Nanocellulose reinforced rubber

The first recorded descriptions of elastomers date from approximately 500 years ago. At the time, European expeditions first encountered rubbers and latex in America. Today, around 2500 plant species are known to produce latex, but the Hevea brasiliensis tree, from the Amazon rainforest, is the only commercially relevant source [191]. This latex is the source of almost all commercially produced NR, which is applied in more than 50,000 products including adhesives, tires, gloves, condoms, and

Nanocellulose reinforced thermoset composites

Thermosets are hard, stiff cross-linked materials that neither soften nor become moldable when heated. The highly cross-linked structure produced by chemical bonds in thermoset materials is directly responsible for the high mechanical and physical strength compared to those of thermoplastics or elastomers. Although thermoset polymers are widely used for engineering components, adhesives, and matrices for fiber-reinforced composites because they have better mechanical properties compared to

Electrospun nanocellulose composites

Electrospinning provides a versatile approach to produce fibers of exceptional length, ranging from 100 nm to several micrometers, uniform in diameter, and diverse in composition [295]. The electrospinning process involves the use of a high voltage to induce the formation of a liquid jet. In this process, a solid fiber is generated as the electrified jet, comprising a highly viscous polymer solution, is continuously stretched by the electrostatic repulsion between surface charges and solvent

Future perspective and application

Being completely renewable, safer to handle, and cheaper to produce, nanocellulose materials possess exceptional physical and chemical properties. The nanocellulose is considered as a viable alternative to the more expensive high tech materials such as carbon fibers and carbon nanotubes. With appropriate conversion and extraction technologies, as well as modification and characterization, nanocellulose can be integrated into bio-based products. Nanocellulose is being developed for use in

Conclusion

The present review reports advances in the uses of CNC and CNF as reinforcement materials in polymer composites. It provides knowledge to stimulate future research in this area. It has been shown that, in the last 10 years, significant developments have occurred in the area of cellulose nanocomposites. Because of the hydrophilicity of nanocellulose, use of the material as reinforcement in polymeric and non-water-soluble polymers is limited. However, the hydroxyl groups on the surface of the

Acknowledgments

The authors, Ishak Ahmad and Hanieh Kargarzadeh, would like to thank the Universiti Kebangsaan Malaysia (UKM) and Ministry of Higher Education of Malaysia (MOHE) for providing research grants, GUP-2016-009 and DIP-2016-026 respectively, to make this research possible.

Hanieh Kargarzadeh is a post-doctoral researcher at the University Kebangsaan Malaysia (UKM) in Selangor, Malaysia. She received her MSc in organic chemistry from Islamic Azad University of Gachsaran, Iran, in 2007 and completed her PhD at University Kebangsaan Malaysia, in 2013. Dr. Kargarzadeh has published a number of papers in high quality international journals and has been involved in a number of books as the author for different chapters. Her research interests lie in the area of

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  • Cited by (0)

    Hanieh Kargarzadeh is a post-doctoral researcher at the University Kebangsaan Malaysia (UKM) in Selangor, Malaysia. She received her MSc in organic chemistry from Islamic Azad University of Gachsaran, Iran, in 2007 and completed her PhD at University Kebangsaan Malaysia, in 2013. Dr. Kargarzadeh has published a number of papers in high quality international journals and has been involved in a number of books as the author for different chapters. Her research interests lie in the area of preparation, characterization and applications of nanocellulose, polymer composite and nanocomposites, and polymer blending.

    Ishak Ahmad is Professor at the School of Chemical Sciences and Food Technology, University Kebangsaan Malaysia (UKM), as well as Head of the Nanocrystalline Research Consortia, under National Nanotechnology Directorate (NND), Malaysia. Prof. Ahmad has authored more than hundred research papers in international peer-reviewed journals and proceedings in the area of polymer composites, nanocomposites, polymer blends, polymer recycling and polymer hydrogels. Furthermore, he written 3 books and contributed chapters for various books. Prof. Ahmad holds four patents.

    Marcos Mariano is postdoctoral researcher in Brazilian Center of Research in Energy and Materials (CNPEM). He received his PhD from Université Grenoble-Alpes in 2016. His main research interests concern preparation, characterization and applications of nanocellulose. Holding several publications about nanocellulose nanocomposites and basic particle characterizations, at the moment his research goes towards preparation of hydrogels with potential biomedical applications.

    Professor Dr. Jin Huang is affiliated with School of Chemistry and Chemical Engineering, Southwest University, China. He received the PhD from Wuhan University, and completed postdoctoral research in Institute of Chemistry, Chinese Academy of Sciences. He has worked in Wuhan University of Technology from 2005 to 2015, and carried out some research in Grenoble Institute of Technology in this period. His research interests focuses on “Soft Matter and Nanomaterials”. Especially for the topic of “Developing chemical and physical methodology and technologies to manufacturing green materials from biomass resources”, he has worked on the hig-value and advanced applications of bioplastics, composites and nanocomposites using natural polymers including cellulose, chitin and chitosan, starch, plant proteins etc.. The progress on surface chemical modification and new nanocomposites of cellulose nanocrystals is worthy of note. Up to now, he has authored and co-authored more than 140 peer-reviewed journal publications, 1 monograph titled as “Polysaccharide-Based Nanocrystals: Chemistry and Applications” and 7 book chapters, over 40 granted China patents, and many conference papers/presentations.

    Ning Lin is associate professor in Department of Chemistry and Life Science and Technology of Wuhan University of Technology, China. He received his PhD at the International School of Paper, Print Media and Biomaterials (Pagora) at University of Grenoble Alpes in France and continued the one-year post-doctoral research. After his MS study at the Department of Chemical Engineering and Technology in Wuhan University of Technology (WHUT) in China, he was awarded the scholarship under the State Scholarship Fund (Chinese Scholarship Council, CSC) to support his PhD study in France. He has authored 21 scientific publications, 1 co-authored book and 6 patents. His research interests include chemical modification, design and development of biomass-based nanoparticles (nanocellulose, nanochitin, starch nanocrystals) and functional applications.

    Alain Dufresne received his Ph.D. in 1991 from INSA Toulouse (Electronics) and was then Post-doc at Polytechnique Montreal, and Lecturer at INSA Lyon. He was appointed Associate Professor in 1993, and then Professor in 2001, at Grenoble University. He is since 2003 Professor at Grenoble INP. He was visiting Professor at UFRJ and Embrapa Fortaleza (Brazil), and UKM (Malaysia). His research interests are the processing and characterization of renewable nanocomposites. He has published +250 peer-reviewed papers. He received the 2016 International Nanotechnology Division Award and FiberLean® Technologies Prize awarded by TAPPI and is in the 2016 top 300 most cited researchers in materials science and engineering/ Elsevier Scopus Data.

    Sabu Thomas is the Director of the International and Interuniversity Centre for Nanoscience and Nanotechnology as well as full professor of Polymer Science and Technology at the School of Chemical Sciences of the Mahatma Gandhi University in Kottayam, India. His research interests include polymer nanocomposites, polymer blends, green bionanotechnological and nano-biomedical sciences. Prof. Thomas has authored more than 600 peer reviewed publications, reviews and book chapters, co-edited 30 books and holds four patents. Furthermore, he has received a number of national and international awards, including a Fellowship of the Royal Society of Chemistry, MRSI award, CRSI award, the Distinguished Professorship award form Josef Stefan Institute, Slovenia, and the Sukumar Maithy award.

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