The highly contemplated disordered regions on native cellulose microfibrils are frequently said to be “alternating” with crystalline regions, distributed along the fibril; however, the exact location and nature of these dislocations has not been completely discerned. Current research on nanocelluloses is limited to highly crystalline cellulose nanocrystals (CNC) and cellulose nanofibers (CNF), without studies on the contribution of disordered cellulose. Recent research on a novel type of nanocelluloses, namely hairy cellulose nanocrystals (HCNC), has demonstrated that a unique two-step oxidation procedure is able to partially preserve disordered cellulose in the form of highly functional “hairs” protruding from each end of a crystalline body. This work aims to understand the location and periodicity of disordered cellulose, as well as the modification and tunable self-assembly via top-down and bottom-up approaches to leverage versatile and superior nanomaterials. In the top-down approach, preferential oxidation of disordered cellulose in various lignocellulosic materials is conducted to form highly functional lignocellulosic micro- and nano-structured materials with charge contents as high as 6 mmol g<sup>-1</sup>. Using the chemistry utilized to form HCNC, selective labeling of disordered cellulose in native microfibrils with gold nanoparticles is then investigated to elucidate the location and periodicity of disordered regions. This enables the bottom-up approach, for the end-to-end self-assembly of disordered cellulose chains in HCNC, leveraging extended and stimuli-responsive networks made up of entirely nanocellulose for the next generation of sustainable materials.

Investigation and chemical modification of disordered cellulose in fibrils: Top-down and bottom-up approaches

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ACS Fall 2022

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