Cellulose nanocrystals in the development of biodegradable materials: A review on CNC resources, modification, and their hybridization

The escalating demand for sustainable materials has propelled cellulose into the spotlight as a promising alternative to petroleum-based products. As the most abundant organic polymer on Earth, cellulose is ubiquitous, found in plants, bacteria, and even a unique marine animal—the tunicate. Cellulose polymers naturally give rise to microscale semi-crystalline fibers and nanoscale crystalline regions known as cellulose nanocrystals (CNCs). Exhibiting rod-like structures with widths spanning 3 to 50 nm and lengths ranging from 50 nm to several microns, CNC characteristics vary based on the cellulose source. The degree of crystallinity, crucial for CNC properties, fluctuates between 49 and 95 % depending on the source and synthesis method. CNCs, with their exceptional properties such as high aspect ratio, relatively low density (≈1.6 g cm−3), high axial elastic modulus (≈150 GPa), significant tensile strength, and birefringence, emerge as ideal candidates for biodegradable fillers in nanocomposites and functional materials. The percolation threshold, a mathematical concept defining long-range connectivity between filler and polymer, governs the effectiveness of reinforcement in nanocomposites. This threshold is intricately influenced by the aspect ratio and molecular interaction strength, impacting CNC performance in polymeric and pure nanocomposite materials. This comprehensive review explores diverse aspects of CNCs, encompassing their derivation from various sources, methods of modification (both physical and chemical), and hybridization with heterogeneous fillers. Special attention is devoted to the hybridization of CNCs derived from tunicates (TCNC) with those from wood (WCNC), leveraging the distinct advantages of each. The overarching objective is to demonstrate how this hybridization strategy mitigates the limitations of WCNC in composite materials, offering improved interaction and enhanced percolation. This, in turn, is anticipated to elevate the reinforcing effects and pave the way for the development of nanocomposites with tunable viscoelastic, physicochemical, and mechanical properties.