Green acid-free one-step hydrothermal ammonium persulfate oxidation of viscose fiber wastes to obtain carboxylated spherical cellulose nanocrystals for oil/water Pickering emulsion

Textile manufacturing industries produce large amounts of viscose fiber wastes (VFW), causing serious environmental pollution. This study presents an acid-free approach to prepare spherical cellulose nanocrystals (SCNs) with carboxyl groups from industrial VFW by one-step hydrothermal ammonium persulfate (APS) oxidation. Novel double-response surface methodology was employed to optimize the reaction conditions. A maximum yield (37.89%) of carboxylated SCN was obtained at reaction time of 4 h, APS concentration of 1 M and temperature of 80 °C, while the SCNs showed gradual size reductions along with increase of carboxyl contents as reaction time and APS concentration increased. Interestingly, it was possible to obtain carboxylated SCNs in only 2 h of reaction with an increase of 16.5% in the crystallinity index, which was attributed to efficient swelling of cellulose chains and oxidation interaction of surface groups under hydrothermal condition. Compared with SCN-2 h, the crystallinity index and maximum degradation temperature of SCN-10 h were improved by 5.5% and 17.9 °C, respectively. Moreover, SCN-10 h exhibited excellent emulsifying capacity to stabilize soybean oil/water Pickering emulsion droplets and emulsion volume were increased with decreased mean diameter of emulsion droplets as SCN-10 h concentration increased. These results indicate that VFW is an attractive source to produce carboxylated SCNs by APS oxidation, making SCN extraction as value-added alternatives to recycle this waste. Such carboxylated SCNs have great potentials as green food Pickering emulsion stabilizers and nanofillers in high-performance composites.