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 utilization of cellulose to its full potential is constrained by its recalcitrance to dissolution resulting from the rigidity of polymeric chains, high crystallinity, high molecular weight, and extensive intra- and intermolecular hydrogen bonding network. Therefore, pretreatment of cellulose is usually considered as a step that can help facilitate its dissolution. We investigated the use of microwave oxygen plasma as a pre-treatment strategy to enhance the dissolution of cotton fibers in aqueous NaOH/Urea solution, which is considered to be a greener solvent system compared to others. Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy, Scanning Electron Microscopy, and Powder X-ray Diffraction analyses revealed that plasma pretreatment of cotton cellulose leads to physicochemical changes of cotton fibers. Pretreatment of cotton cellulose with oxygen plasma for 20 and 40 min resulted in the reduction of the molecular weight of cellulose by 36% and 60% and crystallinity by 16% and 25%, respectively. This reduction in molecular weight and crystallinity led to a 34% and 68% increase in the dissolution of 1% (w/v) cotton cellulose in NaOH/Urea solvent system. Thus, treating cotton cellulose with microwave oxygen plasma alters its physicochemical properties and enhanced its dissolution.

Low-quality cotton fibers, often overlooked as low-value materials, constitute a marginalized waste stream in the cotton industry. This study endeavored to repurpose these fibers into mulch gel films, specifically exploring their efficacy in covering moisture-controlled soil beds. Through a meticulously designed series of processing methods, cellulose/glycerol film was successfully fabricated by regenerating cellulose hydrogels in N,N-dimethylacetamide/lithium chloride solutions, followed by plasticization in glycerol/water solutions and hot pressing. The film was then employed to cover soil beds for a duration of up to 252 days, followed by soil burial assessments. Despite expectations of degradation, the film maintained structural integrity throughout the soil covering period but underwent complete biodegradation after 80 days of soil burial, thereby completing a closed carbon cycle. Intriguingly, both tensile strength and modulus exhibited no diminishment but instead increased after soil covering, contrary to expectations given the usual role of degradation. Mechanistic insights revealed that the removal of glycerol contributed to the mechanical enhancement, while microbial activity predominately decomposed the amorphous regions in soil covering and targeted the crystalline portions in soil burial, elucidating the main biodegradation mechanisms. In summary, this study presents, for the first time, the potential of upcycling low-quality cotton fibers into high-value mulch gel films for agricultural practices within a closed carbon cycle.