With increasing environmental and ecological concerns due to the use of petroleum-based chemicals and products, the synthesis of fine chemicals and functional materials from natural resources is of great public value. Nanocellulose may prove to be one of the most promising green materials of modern times due to its intrinsic properties, renewability, and abundance. In this review, we present nanocellulose-based materials from sourcing, synthesis, and surface modification of nanocellulose, to materials formation and applications. Nanocellulose can be sourced from biomass, plants, or bacteria, relying on fairly simple, scalable, and efficient isolation techniques. Mechanical, chemical, and enzymatic treatments, or a combination of these, can be used to extract nanocellulose from natural sources. The properties of nanocellulose are dependent on the source, the isolation technique, and potential subsequent surface transformations. Nanocellulose surface modification techniques are typically used to introduce e...

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Nanocellulose, a Versatile Green Platform: From Biosources to Materials and Their Applications

We report a study of self-assembled beta-pleated sheets in B. mori silk fibroin films using thermal analysis and infrared spectroscopy. B. mori silk fibroin may stand as an exemplar of fibrous proteins containing crystalline beta-sheets. Materials were prepared from concentrated solutions (2−5 wt % fibroin in water) and then dried to achieve a less ordered state without beta-sheets. Crystallization of beta-pleated sheets was effected either by heating the films above the glass transition temperature (Tg) and holding isothermally or by exposure to methanol. The fractions of secondary structural components including random coils, alpha-helices, beta-pleated sheets, turns, and side chains were evaluated using Fourier self-deconvolution (FSD) of the infrared absorbance spectra. The silk fibroin films were studied thermally using temperature-modulated differential scanning calorimetry (TMDSC) to obtain the reversing heat capacity. The increment of the reversing heat capacity ΔCp0(Tg) at the glass transition fo...

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Determining Beta Sheet Crystallinity in Fibrous Proteins by Thermal Analysis and Infrared Spectroscopy

Cellulose nanocrystals, a class of fascinating bio-based nanoscale materials, have received a tremendous amount of interest both in industry and academia owing to its unique structural features and impressive physicochemical properties such as biocompatibility, biodegradability, renewability, low density, adaptable surface chemistry, optical transparency, and improved mechanical properties. This nanomaterial is a promising candidate for applications in fields such as biomedical, pharmaceuticals, electronics, barrier films, nanocomposites, membranes, supercapacitors, etc. New resources, new extraction procedures, and new treatments are currently under development to satisfy the increasing demand of manufacturing new types of cellulose nanocrystals-based materials on an industrial scale. Therefore, this review addresses the recent progress in the production methodologies of cellulose nanocrystals, covering principal cellulose resources and the main processes used for its isolation. A critical and analytical examination of the shortcomings of various approaches employed so far is made. Additionally, structural organization of cellulose and nomenclature of cellulose nanomaterials have also been discussed for beginners in this field.

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Recent progress in cellulose nanocrystals: sources and production

Nanocellulose, a tiny fiber with huge applications

Cellulose nanocrystals and cellulose nanofibrils based hydrogels for biomedical applications.

This work presents an environmentally friendly, iodine-catalyzed chemical modification method to generate highly hydrophobic, optically active nanocrystalline cellulose (CNC). The high degree of ester substitution (DS = 2.18), hydrophobicity, crystalline behavior, and optical activity of the generated acetylated CNC (Ac-CNC) were quantified by TEM, FTIR, solid 13C NMR, contact angle, XRD, and POM analyses. Ac-CNC possesses substantial enhancement in thermal stability (16.8%) and forms thin films with an interlayer distance of 50–150 nm, presenting cavities suitable for entrapping nano- and microparticles. Generated Ac-CNC proved to be an effective reinforcing agent in hydrophobic polymer matrices for fabricating high performance nanocomposites. When integrated at a very low weight percentage (0.5%) in an epoxy matrix, Ac-CNC provided for a 73% increase in tensile strength and a 98% increase in modulus, demonstrating its remarkable reinforcing potential and effective stress transfer behavior. The method of...

Highly Modified Cellulose Nanocrystals and Formation of Epoxy-Nanocrystalline Cellulose (CNC) Nanocomposites

Recombinant exon-encoded resilins for elastomeric biomaterials.

This research explores the properties of bionanocomposite films prepared by binding recombinant resilin-like protein (res) consisting of the exon 1 resilin sequence from Drosophila melanogaster, engineered to include a cellulose binding domain (CBD), to cellulose nanocrystals (CNCs). The optimal binding of res-CBD to CNCs was 1:5 by mass, and the resulting res-CBD-CNCs remained colloidally stable in water. Res-CBD-CNCs were solvent cast into transparent, free-standing films, which were more hydrophobic than neat CNC films, with water contact angles of 70–80° compared to 35–40° for the latter. In contrast to the multi-domain orientation typical of chiral nematic CNC films, res-CBD-CNC and CBD-CNC films exhibited long-range, uniaxial orientation that was apparently driven by the CBD moiety. Glycerol was studied as an additive in the films to determine whether the addition of a wet component to solvate the recombinant protein improved the mechanical properties of the res-CBD-CNC films. In comparison...

Bionanocomposite Films from Resilin-CBD Bound to Cellulose Nanocrystals

Development of high-performance bio-nanocomposite adhesives is of high interest due to their environmentally friendly nature and superior mechanical properties in outdoor environments. Nano-crystalline cellulose (NCC) and resilin are among the most promising bio-nanofillers, providing strength and elasticity, respectively. A novel bio-nanocomposite comprised of NCC and resilin fused to a cellulose binding domain (Res.-CBD) is presented. As a case study, commercial epoxy adhesive was chosen as a matrix for the bio-nanocomposite adhesive. Insertion of hydrophilic NCC into hydrophobic resins, such as epoxy, is typically performed using solvent exchange, chemical modification, emulsifier addition or mixing with water-borne resins, techniques which either limit the material’s application range or which are considered environmentally unfriendly. The unique approach presented here employed Res.-CBD as a surfactant-like agent supportive of the direct insertion of water-suspended NCC into an epoxy resin. The presented approach involves binding of Res.-CBD to NCC through its CBD domain and a chemical reaction between the resin epoxide groups and Res.-CBD amine moieties. The resulting bio-nano material shows a 50 % increase in the Young’s modulus and a 20 % decrease in the tan(δ), compared to pristine epoxy. This novel epoxy adhesive can be advantageous in applications where higher elasticity and Young’s modulus are required.

Amit Rivkin

Papers

Nanocellulose, a tiny fiber with huge applications

Highly Modified Cellulose Nanocrystals and Formation of Epoxy-Nanocrystalline Cellulose (CNC) Nanocomposites

Recombinant exon-encoded resilins for elastomeric biomaterials.

Bionanocomposite Films from Resilin-CBD Bound to Cellulose Nanocrystals

Insertion of nano-crystalline cellulose into epoxy resin via resilin to construct a novel elastic adhesive