Observation of osmotically driven, highly controllable and reconfigurable oil/water phase separation

Liquid-liquid phase separation has been proven to be a valuable method for producing structured materials and creating chemical systems. Although several strategies have been developed to date, osmotically driven oil/water phase separation has never been achieved owing to the limited solubility of inorganic salts in conventional organic solvents and thus the insufficient osmotic driving force to counterbalance the Laplace pressure associated with the interfacial tension. Herein, we report the discovery that a mixture of 1-alkyl-3-vinylimidazolium bis(trifluoromethanesulfonyl)imide and LiTf₂N can generate sufficient and widely tunable osmotic pressure in oil to realize water transport from the surrounding aqueous phase into the oil phase, triggering spontaneous phase separation. This osmotically driven phase separation could be modulated with unprecedented flexibility, offering unlimited possibilities to facilely access diverse thermodynamically metastable structures using one system. Importantly, this oil system can serve as a general phase separation carrier platform for realizing phase separation of various substances.