Effect of Electric Potential and Chain Length on Tribological Performances of Ionic Liquids as Additives for Aqueous Systems and Molecular Dynamics Simulations

As pure lubricants, ILs performed very well by forming the classical self-assembly bilayer at the sliding interface. The interface mechanism is still not clear in a very polar, e.g., water-based lubricating system. In this work, the interfacial absorption and tribological behavior of carboxylic alkanolamine ionic liquids (CAILs) serving as aqueous lubricating additives were studied by applying positive and negative potentials on the friction pair, accompanied by the comprehensive discussion of data from critical micelle concentration, quartz crystal microbalance, ECR, and MD results. The results reveal that the adsorption behavior, unexpectedly, was affected by the high polarity of H2O, where a less dense double-layer structure is observed at the interface by model imitation. Conversely, the monomolecular adsorption layer constructed electrostatically between the polar head (−COO–) and the positive base dominates the tribofilm. Meanwhile, the cations are partially accumulating around anions in the presence of static electricity, which does not form a neat and dense one-to-one corresponding cation–anion pair. In the solution, the IL maintains a state of dissociation and minor agglomeration. Furthermore, an increase in alkyl chains contributes to the thickness of the protective film generated by CAILs on the sliding asperity. Eventually, the synergistic effect from physical adsorption and the tribochemical reaction is responsible for excellent lubricity and antiwear performance of CAILs.