Highly Concentrated Electrolyte Superlubricants Enhanced by Interfacial Water Competition Around Chemically Active MgO Additives.

The low concentration of water-based lubricants and the high chemical inertness of the additives involved are often regarded as basic norms in the design of liquid lubricants. Herein, a novel liquid superlubricant of an aqueous solution containing a relatively high concentration of salt, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), is reported for the first time, and the superlubricity stability and load-bearing capacity of the optimized system (MgO 0.10 /LiTFSI 10 ) are effectively strengthened by the addition of only trace (0.10 wt %) water-chemically active MgO additives. It demonstrates higher applicable loads, lower COF (∼0.004), and stability relative to the base solution. Only a trace amount of MgO additive is needed for the superlubricity, which makes up for the cost and environmental deficiencies of LiTFSI 10 . The weak interaction region between free water and the outer-layer water of Li + hydration shells becomes a possible ultralow shear resistance sliding interface; the Mg(OH) 2 layer, generated by the reaction of MgO with water, further creates additional weakly interacting interfaces, leading to the formation of an asymmetric contact between the clusters/particles within the hydrodynamic film by moderating the competition between interfacial water and free water, thus achieving high load-bearing macroscopic superlubricity. This study deepens the contribution of electrolyte concentration to ionic hydration and superlubricity due to the low shear slip layer formed by interfacial water competition with water-activated solid additives, providing new insights into the next generation of high load-bearing water-based liquid superlubricity systems.