Finding renewable alternatives to the commonly used reinforcement materials in composites is attracting a significant amount of research interest. Nanocellulose is a promising candidate owing to its wide availability and favorable properties such as high Young’s modulus. This study addressed the major problems inherent to cellulose nanocomposites, namely, controlling the fiber structure and obtaining a sufficient interfacial adhesion between nanocellulose and a non-hydrophilic matrix. Unidirectionally aligned cellulose nanofiber filament mats were obtained via ice-templating, and chemical vapor deposition was used to cover the filament surfaces with an aminosilane before impregnating the mats with a bio-epoxy resin. The process resulted in cellulose nanocomposites with an oriented structure and a strong fiber–matrix interface. Diffuse reflectance infrared Fourier transform and X-ray photoelectron spectroscopy studies revealed the presence of silane on the filaments. The improved interface, resulting from the surface treatment, was observable in electron microscopy images and was further confirmed by the significant increase in the tan delta peak temperature. The storage modulus of the matrix could be improved up to 2.5-fold with 18 wt% filament content and was significantly higher in the filament direction. Wide-angle X-ray scattering was used to study the orientation of cellulose nanofibers in the filament mats and the composites, and the corresponding orientation indices were 0.6 and 0.53, respectively, indicating a significant level of alignment.

Large amounts of cellulose-based waste textiles are generated every year, yet little is done to recycle this waste. Alternatives such as fiber-to-fiber recycling, where a significant part of the value of the waste textiles is recovered, are attractive possibilities. In this study, we have investigated the viability of using hydrated zinc chloride (ZnCl₂·4H₂O) as a solvent and swelling agent to convert cotton waste textiles (the most abundant cellulose-based waste textile) into a dissolving pulp that can be used as raw material for the production and spinning of viscose fibers. The solvent produced an accessible dissolving pulp and exhibited excellent recyclability, maintaining good dissolving power even after repeated recycling. The dissolving pulp was subsequently used to produce viscose dope, a spinning solution which was spun and cut into viscose staple fibers. The viscose dope exhibited good properties (moderate filter clogging value and gamma number), and the resulting staple fibers were strong and of good quality (high linear density, elongation, and tenacity). These results illustrate the potential of using hydrated zinc chloride for the production of viscose grade dissolving pulp from cotton waste textiles.

The fashion industry is becoming one of the largest emitters worldwide due to its high consumption of raw materials, its effluents, and the fact that every garment will eventually contribute to the vast amount of waste being incinerated or accumulating in landfills. Although fiber-to-fiber recycling processes are being developed, the mechanical properties of the textile fibers are typically degraded with each such recycle. Thus, tertiary recycling alternatives where textiles are depolymerized to convert them into valuable products are needed to provide end-of-life alternatives and to achieve circularity in the fashion industry. We have developed a method whereby cotton waste textiles are depolymerized to form a glucose solution, using sulfuric acid as the sole catalyst, with a high yield (>70%). The glucose solution produced in this process has a high concentration (>100 g/L), which reduces the purification cost and makes the process industrially relevant. This method can be applied regardless of the quality of the fibers and could therefore process other cellulosic fibers such as viscose. The glucose produced could subsequently be fermented into butanediol or caprolactam, precursors for the production of synthetic textile fibers, thus retaining the value of the waste textiles within the textile value chain.

The orientation of polymer composites is one way to increase the mechanical properties of the material in a desired direction. In this study, the aim was to orient chitin nanocrystal (ChNC)-reinforced poly(lactic acid) (PLA) nanocomposites by combining two techniques: calendering and solid-state drawing. The effect of orientation on thermal properties, crystallinity, degree of orientation, mechanical properties and microstructure was studied. The orientation affected the thermal and structural behavior of the nanocomposites. The degree of crystallinity increased from 8% for the isotropic compression-molded films to 53% for the nanocomposites drawn with the highest draw ratio. The wide-angle X-ray scattering results confirmed an orientation factor of 0.9 for the solid-state drawn nanocomposites. The mechanical properties of the oriented nanocomposite films were significantly improved by the orientation, and the pre-orientation achieved by film calendering showed very positive effects on solid-state drawn nanocomposites: The highest mechanical properties were achieved for pre-oriented nanocomposites. The stiffness increased from 2.3 to 4 GPa, the strength from 37 to 170 MPa, the elongation at break from 3 to 75%, and the work of fracture from 1 to 96 MJ/m³. This study demonstrates that the pre-orientation has positive effect on the orientation of the nanocomposites structure and that it is an extremely efficient means to produce films with high strength and toughness.

Silica nanoparticles (SNPs) dissolve in alkaline media, which limits their use in certain applications. Here, we report a delayed dissolution of SNPs in strong alkali induced by zinc oxide (ZnO), an additive which also limits gelation of alkaline cellulose solutions. This allows incorporating high solid content of silica (30 wt%) in cellulose solutions with retention of their predominant viscous behavior long enough (ca. 180 min) to enable fiber wet spinning. We show that without addition of ZnO, silica dissolves completely, resulting in strong gelation of cellulose solutions that become unsuitable for wet spinning. With an increase of silica concentration, gelation of the solutions occurs faster. Employing ZnO, silica-rich regenerated cellulose fibers were successfully spun, possessing uniform cross sections and smooth surface structure without defects. These findings are useful in advancing the development of functional man-made cellulose fibers with incorporated silica, e.g., fibers with flame retardant or self-cleaning properties.

In this study, the possibility of adding nanocellulose and its dispersion to polyamide 6 (PA6), a polymer with a high melting temperature, is investigated using melt extrusion. The main challenges of the extrusion of these materials are achieving a homogeneous dispersion and avoiding the thermal degradation of nanocellulose. These challenges are overcome by using an aqueous suspension of never-dried nanocellulose, which is pumped into the molten polymer without any chemical modification or drying. Furthermore, polyethylene glycol is tested as a dispersant for nanocellulose. The dispersion, thermal degradation, and mechanical and viscoelastic properties of the nanocomposites are studied. The results show that the dispersant has a positive impact on the dispersion of nanocellulose and that the liquid-assisted melt compounding does not cause the degradation of nanocellulose. The addition of only 0.5 wt.% nanocellulose increases the stiffness of the neat polyamide 6 from 2 to 2.3 GPa and shifts the tan δ peak toward higher temperatures, indicating an interaction between PA6 and nanocellulose. The addition of the dispersant decreases the strength and modulus but has a significant effect on the elongation and toughness. To further enhance the mechanical properties of the nanocomposites, solid-state drawing is used to create an oriented structure in the polymer and nanocomposites. The orientation greatly improves its mechanical properties, and the oriented nanocomposite with polyethylene glycol as dispersant exhibits the best alignment and properties: with orientation, the strength increases from 52 to 221 MPa, modulus from 1.4 to 2.8 GPa, and toughness 30 to 33 MJ m⁻³ in a draw ratio of 2.5. This study shows that nanocellulose can be added to PA6 by liquid-assisted extrusion with good dispersion and without degradation and that the orientation of the structure is a highly-effective method for producing thermoplastic nanocomposites with excellent mechanical properties.