Characterization of Type-II Acetylated Cellulose Nanocrystals with Various Degree of Substitution and Its Compatibility in PLA Films

In order to decrease the self-agglomeration and improve the hydrophobic properties of type-II acetylated cellulose nanocrystals (ACNC II), various degree of substitution (DS) values of ACNCs were successfully prepared by a single-step method from microcrystalline cellulose with anhydrous phosphoric acid as the solvent, and acetic anhydride as the acetylation reagent, under different reaction temperatures (20–40 °C). To thoroughly investigate the DS values of ACNC II, analyses were performed using Fourier transform infrared spectroscopy (FT-IR), (13)C cross polarization-magic angle spinning (CP-MAS) nuclear magnetic resonance (NMR), and X-ray photoelectron spectroscopy (XPS). At a reaction temperature of 40°C, the highest DS value was successfully obtained. XRD proved that the crystal structure of ACNC II with various DS values was maintained after acetylation. TEM showed the threadlike shape for ACNC II with various DS values. The ACNC II with various DS values was introduced into a polylactic acid (PLA) matrix to produce PLA/ACNC composite films, which showed improved rheological and thermal properties. This improvement was primarily attributed to good dispersion of the ACNC II, and the interfacial compatibility between ACNC II and the PLA matrix. This study aims to analyze the compatibility of ACNC II with various DS values in the PLA matrix by microstructure, crystallization, and rheological and thermal tests.