Chiral Self-Assembly Behavior of Carboxylated Cellulose Nanocrystals Isolated by Recyclable Oxalic Acid from Degreasing Cotton

Carboxylated cellulose nanocrystals (OA-CNCs) isolated by aqueous recyclable oxalic acid hydrolysis from degreasing cotton were used to observe its self-assembly behavior and chiral nematic properties. The oxalic acid here served as the sole catalyst to esterify and hydrolyze the degreasing cotton. The results indicated that the obtained OA-CNC suspensions were spontaneously phase-separated into a chiral nematic mesophase above a critical concentration, and the occurrence of chiral self-assembly is highly dependent on the aspect ratio and the surface charge of the OA-CNC suspension. Scanning electron microscopy images of the cross section of OA-CNC solid films revealed a periodic ordered multilayer structure. The residual OA was easily recovered through simple re-crystallization method after reactions with a high recovery rate of at least 90%. The recycled OA (ROA) had excellent performance in terms of ROA-CNC yield even after reusing for five cycles. Moreover, the resultant ROA-CNCs from recycled OA could also form chiral nematic ordered phases with little change in the critical concentration and pitch, suggesting excellent suitability for sustainable OA-CNC production for photonics and other specialty applications.