Novel insights on room temperature-induced cellulose dissolution mechanism via ZnCl2 aqueous solution: Migration, penetration, interaction, and dispersion.

The unique molecular structure of cellulose makes it challenging to dissolve at room temperature (R.T.), and the dissolution mechanism remains unclear. In this study, we employed ZnCl2 aqueous solution for cellulose dissolution at R.T., proposing a novel four-stage dissolution mechanism. The efficient dissolution of cellulose in ZnCl2 aqueous solution at R.T. involves four indispensable stages: rapid migration of hydrated Zn2+ ions towards cellulose, sufficient penetration between cellulose sheets, strong interaction with cellulose hydroxyl groups, and effective dispersion of separated cellulose chains. The proposed four-stage dissolution mechanism was validated through theoretical calculations and experimental evidence. The hydrated Zn2+ ions in ZnCl2 + 3.5H2O solvent exhibited ideal migration, penetration, interaction, and dispersion abilities, resulting in efficient cellulose dissolution at R.T. Moreover, only slight degradation of cellulose occurred in ZnCl2 + 3.5H2O at R.T. Consequently, the regenerated cellulose materials obtained from ZnCl2 + 3.5H2O (R.T.) exhibited better mechanical properties. Notably, the solvent recovery rate reached about 95 % based on previous usage during five cycles. The solvent is outstanding for its green, low-cost, efficiency, simplicity, R.T. conditions and recyclability. This work contributes to a better understanding of the cellulose dissolution mechanisms within inorganic salt solvents at R.T., thereby guiding future development efforts towards greener and more efficient cellulosic solvents.