Comparative analysis of millet bran nanocelluloses with various morphologies: Revealing differences in the formation mechanism and structure characteristics

Abstract

To investigate the differences of nanocelluloses with various morphologies, ammonium persulphate (APS) oxidation, H3PO4 dissolution and regeneration, and ball milling combined with 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) as a medium were applied to isolate cellulose nanocrystals (MCNCs), cellulose nanospheres (MCNSs) and cellulose fibrils (MCNFs) from millet bran. The structure, properties, and formation mechanism of three nanocelluloses were comparatively investigated by Fourier transform infrared spectroscopy, X-ray diffraction, thermogravimetric analysis, atomic force microscope, scanning electronic microscope, and emulsifying ability evaluation. MCNCs had needle-like structures due to the removal of amorphous regions, MCNFs appeared fibrous structures due to swelling and mechanical force, and MCNSs displayed spherical structures through self-assembly. MCNCs and MCNFs were confirmed to exhibit cellulose I structures with crystallinities of 61.24 % and 50.09 %, respectively. MCNSs showed the highest crystallinity of 68.41 % with a cellulose II structure. MCNFs and MCNSs exhibited higher initial decomposition temperatures, while MCNCs showed the highest residual mass. MCNFs suspension showed the highest apparent viscosity, while MCNSs suspension demonstrated superior dispersion. MCNSs-emulsion displayed the smallest droplet size, and MCNFs-emulsion exhibited the highest viscosity. This study reveals the formation mechanisms and relationship between morphologies and properties of three millet bran nanocelluloses, providing a theoretical basis for their application.