Molecular partitioning in ternary solutions of cellulose

Neutron scattering measurements on the structure and dynamics of ternary solutions of microcrystalline cellulose (MC) in mixtures of an ionic liquid (IL) 1-ethyl-3-methylimidazolium acetate and a polar organic solvent dimethylformamide (DMF) have shown that MC can be fully dissolved in solvent mixtures. Data also show the molecular partitioning of IL into coexisting states. The structure partitioning is manifested as IL adsorbed to cellulose molecules with additional IL self-assembled to form clusters in solution, while the dynamics partitioning shows dynamical heterogeneities of the IL with slow dynamics resembling neat IL and fast dynamics being coupled with the solvent. The composition dependence of the molecular partitioning results in a solubility gap in dilute cellulose solutions and a phase boundary criterion of the molar ratio of IL / MC similar to 3 in more concentrated regimes. The two characteristics together define the main features of the dissolution phase diagram of ternary cellulose mixtures of MC / IL / DMF at the room temperature.