A Review on Cellulose Nanocrystals As Promising Biocompounds for the Synthesis of Nanocomposite Hydrogels
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Accepted Manuscript Title: A review on cellulose nanocrystals as promising biocompounds for the synthesis of nanocomposite hydrogels Authors: Jamileh Shojaeiarani, Dilpreet Bajwa, Alimohammad Shirzadifar PII: S0144-8617(19)30417-5 DOI: https://doi.org/10.1016/j.carbpol.2019.04.033 Reference: CARP 14807 To appear in: Received date: 17 January 2019 Revised date: 10 March 2019 Accepted date: 7 April 2019 Please cite this article as: Shojaeiarani J, Bajwa D, Shirzadifar A, A review on cellulose nanocrystals as promising biocompounds for the synthesis of nanocomposite hydrogels, Carbohydrate Polymers (2019), https://doi.org/10.1016/j.carbpol.2019.04.033 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. A review on cellulose nanocrystals as promising biocompounds for the synthesis of nanocomposite hydrogels Jamileh Shojaeiarania,*, Dilpreet Bajwab, Alimohammad Shirzadifarc *Corresponding Author a Department of Mechanical Engineering, North Dakota State University, Fargo, ND 58102, United States Email: [email protected] , Phone: +1-701-799-7759, ORCID: 0000-0002-1882-0061 b Department of Mechanical Engineering, North Dakota State University, Fargo, ND 58102, United States Email: [email protected] , Phone: +1-701-231-7279 ORCID: 0000-0001-9910-8035 c Department of Agricultural and Biosystems Engineering, North Dakota State University, Fargo, ND, USA Email: [email protected] , Phone: +1-701-799-7780 Highlights ACCEPTED The application of hydrogels containing MANUSCRIPT CNCs are intensively studied. Specific studies on biomedical application of CNC hydrogels are described. Synthesis methods of hydrogels containing CNCs are covered. CNC hydrogels with high adsorption capacity to positive ions are reviewed. 1 ABSTRACT Hydrogels are hydrophilic cross-linked polymer networks formed via the simple reaction of one or more monomers with the ability to retain a significant extent of water. Owing to an increased demand for environmentally friendly, biodegradable, and biocompatible products, cellulose nanocrystals (CNCs) with high hydrophilicity have emerged as a promising sustainable material for the formation of hydrogels. The cytocompatibility, swellability, and non-toxicity make CNC hydrogels of great interest in biomedical, biosensing, and wastewater treatment applications. There has been a considerable progress in the research of CNC hydrogels, as the number of scientific publications has exponentially increased (>600%) in the last five years. In this paper, recent progress in CNC hydrogels with particular emphasis on design, materials, and fabrication techniques to control hydrogel architecture, and advanced applications are discussed. List of Abbreviations Abbreviation Stands for CNCs Cellulose nanocrystals AA Acrylic acid HEMA Hyderoxy ethyl methacrylate MBA N,N'‐ methylenebisacrylamide PAA Poly(acrylic acid) KPS Potassium persulfate ACCEPTEDGQDs Graphene quantum MANUSCRIPT dots PEG Polyethylene glycol PAM Polyacrylamide HA Hyaluronic acid 2 QXH Quaternized xylan CAA Cellulose acetoacetate PVA Polyvinyl alcohol GO Graphene oxide PMC Polyacrylamide-sodium carboxymethylcellulose SA Sodium alginate SG Silica glass HPCS Hydroxypropyl chitosan GDL Glucono-δ-lactone PNIPAAm Poly(N-isopropyl acrylamide) MB Methylene blue CS Chitosan Keywords: Cellulose nanocrystals hydrogel; Nanomaterials; Biomedical application; Biosensor; Wastewater treatment. 1. Introduction Rising concerns regarding the negative impact of petroleum-based polymers on the environment, and the potential applications of biopolymers calls for a transition from petroleum- based polymers to sustainable and renewable ones. Such a transition imposes a substantial challenge for scientists and industries requiring innovative alternatives and the applicable methods improving the potential application of materials. With the emergence and progress of nanotechnology, hydrogels, a special form of bulk materials, have received much attention owing to ACCEPTEDtheir unique and excellent moisture retention MANUSCRIPT characteristics. Hydrogels are 3D network colloidal gels formed through cross-linking of hydrophilic polymer chains (Nair et al., 2019) with the ability of absorbing and retaining large volumes of water in an aqueous environment, without itself dissolving in water (Mondal & Haque, 2019). 3 The hydrophilic nature of hydrogel component governs the water sorption, and the swelling response of the hydrogels in the swollen stage is attributed to the large free space between cross- linked networks (Olad, Zebhi, Salari, Mirmohseni, & Tabar, 2018). Hydrogels were introduced by Wichterle for the first time in 1960 through a cross-linked hydroxyethyl methacrylate (HDMA) (Otto & Drahoslav, 1960). Thereafter, hydrogels have received a significant amount of attention in different areas such as agriculture (Pakdel & Peighambardoust, 2018), waste management (T. Singh & Singhal, 2018), and stimuli-responsive sensors and actuators (M. Li et al., 2018; Nam et al., 2018). Synthetic hydrogels used to be of great importance due to high processability, high water uptake, long service life, and the wide range of raw chemical resources (Zia et al., 2017). However, the use of these types of hydrogels imposed a significant economic and environmental burden on the society and remained a leading cause of global dependence on petroleum-based polymers. Synthetic hydrogels such as polyethylene glycol (PEG), polyvinyl alcohol (PVA), and polyvinyl pyrrolidone (PVP) are formed via chemical polymerization from man-made monomers. Synthetic hydrogels are difficult to biodegrade, and causes environmental damages such as oxygen demand (González, Agostini, & Milrad, 2008), septic systems and landfills (Julinová, Vaňharová, & Jurča, 2018). In addition, the application of petroleum-based polymers is tied to the negative impact to economy since the price of the petroleum in the international market is fluctuating over years, and this inspires researchers and industries into the field of biopolymer research. Particularly, public awareness, social trends and technological advancement in bio-based materialsACCEPTED has gradually increased the application MANUSCRIPT of natural hydrogels in commercial fields. Bio- based hydrogels exhibit a diverse application in biomedical area such as cell therapeutics, wound dressing (Ge et al., 2018), and tissue engineering (X. Yang et al., 2018) due to their inherent non- 4 toxicity, biocompatibility, and highly hydrated three-dimensional porous structure. So far, a wide range of materials (both natural and synthetic) has been examined for the fabrication of hydrogels. Table 1 provides a comparative account of the properties of some of the commonly used polymers for preparing biocomposite hydrogels. Table 1. Properties of some commonly used materials for biocomposite hydrogels fabrication. Bio-based Key properties Limitations Application References material Adsorbent for Fragile and low Biocompatible, heavy metals, (Aderibigbe & Buyana, 2018) Alginate stretchability, weak biodegradable, pH sensitive drug delivery, (Yi et al., 2018) absorbing capacity wound dressing Antimicrobial activity, antistatic activity, nontoxic, Low mechanical Wound dressing, (Khorasani, Joorabloo, Chitosan deodorizing property, strength, poor water drug delivery, Moghaddam, Shamsi, & chemical reactivity, cost- resistance cartilage repair MansooriMoghadam, 2018) effectiveness (Lou, Stowers, Nam, Xia, & High rate of stress Drug delivery, Cellular affinity, tissue Chaudhuri, 2018; H.-S. Yu, Collagen relaxation, weak cell culture, tissue compatibility Lee, Seo, Knowles, & Kim, and viscoelastic gel engineering 2015) Low capacity and Slow release of Antioxidant, antifungal, weak selectivity in hydrophilic drugs, (Thakur & Thakur, 2015; Y. Lignin heavy metals extraction wastewater wastewater Wang et al., 2018) treatment treatment Biocompatibility, Weak gelation Drug delivery, bioresorbability, low Silk performance and tissue (Kim, Kim, Choi, Park, & Ki, immunogenicity, mechanical fibrion low mechanical engineering, cell 2018) resilience, ease of processing strength culture and functionalization Tasteless, hydrophilic, High permeability Wound dressing, biodegradable, insoluble in and low gas barrier, drug delivery, (De France, Hoare, & Cellulose ACCEPTEDwater and most organic weak mechanical MANUSCRIPT waste water Cranston, 2017) solvents, adsorbent properties management Drug delivery, Biocompatibility, and tissue (Goodarzi, Jadidi, Weak mechanical Gelatin biodegradable and non-toxic engineering, Pourmotabed, Sharifi, & properties nature corneal Aghamollaei, 2019) engineering 5 Natural, insoluble protein Weak mechanical Tissue (Gopalakrishnan, Fibrin biocompatibility, properties engineering, drug Shankarappa, & Rajanikant, biodegradability and cell delivery 2019) Cellulose, the most abundant renewable organic material in the world, has been extensively explored for producing new materials, especially in the form of micro or nano-scale with different shape and crystallinity. Cellulose nanocrystals (CNCs), the crystalline regions of cellulose, are extracted from cellulose using top-down