Concentrating Immiscible Molecules at Solid@MOF Interfacial Nanocavities to Drive an Inert Gas-Liquid Reaction at Ambient Conditions

Gas-liquid reactions form the basis of our everyday lives, yet they still suffer poor reaction efficiency and are difficult to monitor insitu, especially at ambient conditions. Now, an inert gas-liquid reaction between aniline and CO2 is driven at 1atm and 298K by selectively concentrating these immiscible reactants at the interface between metal-organic framework and solid nanoparticles (solid@MOF). Real-time reaction SERS monitoring and simulations affirm the formation of phenylcarbamic acid, which was previously undetectable because they are unstable for post-reaction treatments. The solid@MOF ensemble gives rise to a more than 28-fold improvement to reaction efficiency as compared to ZIF-only and solid-only platforms, emphasizing that the interfacial nanocavities in solid@MOF are the key to enhance the gas-liquid reaction. Our strategy can be integrated with other functional materials, thus opening up new opportunities for ambient-operated gas-liquid applications.