Esterification of cellulose using carboxylic acid-based deep eutectic solvents to produce high-yield cellulose nanofibers

Deep eutectic solvents (DESs), as emerging green solvents, provide a new opportunity for the biorefinement of biomass, component extraction, and cellulose nanofibrillation. Herein, different carboxylic acid-based DESs were applied for preparation of cellulose nanofibers (CNFs) from cellulose raw materials accompanied by simultaneous esterification modifications of CNFs. The results showed that pretreatment of DESs combined with mechanical treatment can swell and esterify the cellulose materials, producing CNFs with widths less than 100 nm. The DES pretreatment temperature played important roles in the esterification modifications and nanofibrillation of cellulose. The esterification modifications of cellulose prevented the over-hydrolysis and dissolution of cellulose during the DES pretreatment, guaranteeing CNFs with high yields of 72 %–88 % and maintaining the cellulose I crystal structure. Moreover, the esterified CNFs were used as a reinforcement to prepare CNF-strengthened polylactic acid (PLA) composites. The surface esterification of the CNFs improved their dispersibility and interfacial compatibility with PLA, thereby achieving the mechanical enhancement of CNF/PLA composites.