Unravelling High-Load Superlubricity of Ionic Liquid Analogues by In Situ Raman: Incomplete Hydration Induced by Competitive Exchange of External Water with Crystalline Water.

A high load-carrying capacity is the key to the practicality of liquid superlubricity, but it is difficult to achieve high load and low friction simultaneously by relying solely on a liquid film. Herein, a choline chloride-based ionic liquid analogue (ILA) macroscale superlubricant is first reported by tuning down strong hydrogen bonding in the ILA via introducing 2-10 wt % water, with a high load of 160 MPa and a low coefficient of friction of 0.006-0.008. In situ Raman reveals that competitive exchange between external water and crystalline water induces weak H-bond-dominated incomplete hydration, conferring a low-shear interface and considerable load-carrying capacity inside the lubricant. It is a hydrodynamic lubrication film rather than a tribochemical/physical adsorption film, allowing it to be applied to friction pairs of various materials. This study unveils the principle of water mediation of high-viscosity ILAs and also provides new insights into the design of practical ILA-based superlubrication materials with high load-carrying capacity.