Structure reorganization of cellulose hydrogel by green solvent exchange for potential plastic replacement

Petroleum-based plastics have raised great environmental concerns from the beginning of their production to the end-of-life cycle. It is urgently needed to develop sustainable and green materials with certain plastic properties. Herein, biobased cellulose films are fabricated from low quality cotton cellulose by manipulating its hydrogen bonding network with green solvents. The cellulose is dispersed in inorganic salts (ZnCl₂/CaCl₂) to form ionic hydrogels, and then transformed into tough and flexible films through ethanol exchange and air drying. Without extra hot-pressing treatment, the aggregate structure of cellulose is re-organized with the disruption and re-construction of hydrogen bonds. Benefiting from the densely packed structure and highly in-plane orientation, the cellulose film presents outstanding optical, thermal and mechanical properties. Such cellulose materials hold a potential for plastic replacement in the field of biodegradable packing.