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.

Petroleum-based synthetic plastics play an important role in our life. As the detrimental health and environmental effects of synthetic plastics continue to increase, the renewable, degradable and recyclable properties of cellulose make subsequent products the “preferred environmentally friendly” alternatives, with a small carbon footprint. Despite the fact that the bioplastic industry is growing rapidly with many innovative discoveries, cellulose-based bioproducts in their natural state face challenges in replacing synthetic plastics. These challenges include scalability issues, high cost of production, and most importantly, limited functionality of cellulosic materials. However, in order for cellulosic materials to be able to compete with synthetic plastics, they must possess properties adequate for the end use and meet performance expectations. In this regard, surface modification of pre-made cellulosic materials preserves the chemical profile of cellulose, its mechanical properties, and biodegradability, while diversifying its possible applications. The review covers numerous techniques for surface functionalization of materials prepared from cellulose such as plasma treatment, surface grafting (including RDRP methods), and chemical vapor and atomic layer deposition techniques. The review also highlights purposeful development of new cellulosic architectures and their utilization, with a specific focus on cellulosic hydrogels, aerogels, beads, membranes, and nanomaterials. The judicious choice of material architecture combined with a specific surface functionalization method will allow us to take full advantage of the polymer’s biocompatibility and biodegradability and improve existing and target novel applications of cellulose, such as proteins and antibodies immobilization, enantiomers separation, and composites preparation.

In this study, the biodegradability of cellulose films was evaluated in controlled-moisture soil environments. The films were prepared from low-quality cotton fibers through dissolution in DMAc/LiCl, casting, regeneration, glycerol plasticization, and hot-pressing. Two soil burial degradation experiments were conducted in August 2020 (11th August to 13th October) and March 2021 (24th March to 24th July) under controlled moisture conditions to assess the biodegradation behavior of cellulose films. The films were retrieved from soil beds at seven-day intervals, and morphological and physicochemical changes in the films were investigated. The results indicated that the cellulose films exhibited gradual changes starting on Day 7 and major changes after Day 35. Stereomicroscopy images showed the growth and development of fungal mycelia on the surface of the films, and FTIR spectroscopy confirmed the presence of biomolecules originating from microorganisms. The tensile strength and elongation of cellulose films were significantly reduced by 64% and 96% in the first experiment and by 40% and 94% in the second experiment, respectively, during the degradation period. Degradation also significantly impacted the thermal stability (14% and 16.5% reduction, respectively, in the first and second studies) of the films. The cellulose-based films completely degraded within 63 days in late summer and 112 days in spring. This study demonstrates that, unlike synthetic plastics, films prepared from low-quality cotton fibers can easily degrade in the natural environment.

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 inN,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