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As the most abundant natural polymer, cellulose is a prime candidate for the preparation of both sustainable and economically viable polymeric products hitherto predominantly produced from oil-based synthetic polymers. However, the utilization of cellulose to its full potential is constrained by its recalcitrance to chemical processing. Both fundamental and applied aspects of cellulose dissolution remain active areas of research and include mechanistic studies on solvent–cellulose interactions, the development of novel solvents and/or solvent systems, the optimization of dissolution conditions, and the preparation of various cellulose-based materials. In this review, we build on existing knowledge on cellulose dissolution, including the structural characteristics of the polymer that are important for dissolution (molecular weight, crystallinity, and effect of hydrophobic interactions), and evaluate widely used non-derivatizing solvents (sodium hydroxide (NaOH)-based systems, N,N-dimethylacetamide (DMAc)/lithium chloride (LiCl), N-methylmorpholine-N-oxide (NMMO), and ionic liquids). We also cover the subsequent regeneration of cellulose solutions from these solvents into various architectures (fibers, films, membranes, beads, aerogels, and hydrogels) and review uses of these materials in specific applications, such as biomedical, sorption, and energy uses.

The use of plant-based biomaterials for tissue engineering has recently generated interest as plant decellularization produces biocompatible scaffolds which can be repopulated with human cells. The predominant approach for vegetal decellularization remains serial chemical processing. However, this technique is time-consuming and requires harsh compounds which damage the resulting scaffolds. The current study presents an alternative solution using supercritical carbon dioxide (scCO2). Protocols testing various solvents were assessed and results found that scCO2 in combination with 2% peracetic acid decellularized plant material in less than 4 h, while preserving plant microarchitecture and branching vascular network. The biophysical and biochemical cues of the scCO2 decellularized spinach leaf scaffolds were then compared to chemically generated scaffolds. Data showed that the scaffolds had a similar Young’s modulus, suggesting identical stiffness, and revealed that they contained the same elements, yet displayed disparate biochemical signatures as assessed by Fourier-transform infrared spectroscopy (FTIR). Finally, human fibroblast cells seeded on the spinach leaf surface were attached and alive after 14 days, demonstrating the biocompatibility of the scCO2 decellularized scaffolds. Thus, scCO2 was found to be an efficient method for plant material decellularization, scaffold structure preservation and recellularization with human cells, while performed in less time (36 h) than the standard chemical approach (170 h).

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There is a continuous change in cell wall composition and organization during cotton fiber development. Cotton fiber strength correlates to the molecular weight (MW) and molecular weight distribution (MWD), and organization of cellulose chains in the secondary cell wall. These parameters change drastically during fiber development. This study reports on the MW, MWD, and organization of cellulose in cotton fibers harvested from two cotton cultivars of Gossypium hirsutum L., (Texas Marker-1 and TX55) at different levels of maturity. Fiber dissolution is necessary to estimate the molecular properties of cellulose. Cellulose in mature cotton fibers is larger in MW and highly crystalline and, therefore, poorly dissolves in common solvent systems. To facilitate the dissolution, fibers were first pretreated with 23% sodium hydroxide and then dissolved in a dimethylacetamide/lithium chloride solvent system. Gel permeation chromatography of dissolved fibers indicated that cellulose in both cultivars reaches its maximum MW around 30 days post anthesis. Fourier transform infrared microspectroscopy imaging in the transmission mode indicates changes in cellulose distribution in cotton fibers with fiber development. The distributions of infrared vibrations of cellulose at 897 (β-linkage of cellulose), 1161 (anti-symmetrical C-O-C stretching of cellulose), and 1429 cm−1 (CH2 scissoring of cellulose) provided information on cellulose deposition in intact cotton fibers.

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The use of eco-friendly bioplastics has become a viable solution to reduce the accumulation of petrochemical products in the biosphere and to decrease microplastic contamination. In this study, we used low-quality cotton fibers that lack textile applications to prepare bioplastics. We dissolved cotton fibers in N,N-dimethylacetamide/lithium chloride (DMAc/LiCl) solvent system and converted cellulose solutions to strong, transparent, and flexible films through casting, gelation, regeneration, plasticization, and hot-pressing. Films were characterized using different analytical techniques to evaluate their physicochemical and mechanical properties. Compared to raw cotton cellulose, regenerated and hot-pressed cellulose films showed amorphous structures and excellent tensile characteristics. The physical and mechanical properties of cellulose films, such as deformation recovery, flexibility, homogeneity, elongation, and surface roughness, were significantly improved by means of plasticization and hot-pressing. Because glycerol plasticization increased the surface hydrophilicity of the films, plasma-induced surface grafting of oleic acid imparted hydrophobicity to cellulose films. This study presents a new avenue for using low-quality cotton fibers that are usually sold at a discounted price to produce value-added bioproducts for different applications. Graphic abstract