Understanding the Role of Surface Chemistry in Nanocellulose Kink Formation: A Case Study of TEMPO-Mediated Oxidation

This study found that the sources of cellulose have a significant effect on the parameters related to the kinks present in nanocellulose. During nanocellulose preparation, 2,2,6,6-tetramethylpiperidinyl-1-oxyl (TEMPO)-mediated oxidation induced partial depolymerization on whole cellulose and made the amorphous regions more susceptible to consequent mechanical treatment irrespective of cellulose sources. However, plant cellulose microfibrils were prone to break into shorter nanocellulose with fewer kinks, while bacterial and tunicate cellulose were more likely to bend rather than break, thus leading to the generation of more kinks. The kinks did not show significant effects on the size, crystallinity index, and thermal properties of nanocellulose for each cellulose source, though the kink numbers were positively related to the mechanical performance of nanocellulose. Collectively, this study elucidated the kink formation mechanisms and clarified the effects of kinks on nanocellulose performance, thus providing new insights into understanding the source and behaviors of microdefects present in nanocellulose.