Potential-dependent superlubricity of stainless steel and Au(111) using a water-in-surface-active ionic liquid mixture

Hypothesis
The friction and interfacial nanostructure of a water-in-surface-active ionic liquid mixture, 1.6 M 1-butyl-3-methylimidazolium 1,4-bis-2-ethylhexylsulfosuccinate ([BMIm][AOT]), can be tuned by applying potential on Au(1 1 1) and stainless steel.

Experimental
Atomic force microscopy (AFM) was used to examine the friction and interfacial nanostructure of 1.6 M [BMIm][AOT] on Au(1 1 1) and stainless steel at different potentials.

Findings
Superlubricity (vanishing friction) is observed for both surfaces at OCP+1.0 V up to a surface-dependent critical normal force due to [AOT]− bilayers adsorbing strongly to the positively charged surface thus allowing AFM tip to slide over solution-facing hydrated anion charged groups. High-resolution AFM imaging reveals ripple-like features within near-surface layers, with the smallest amplitudes at OCP+1 V, indicating the highest structural stability and resistance to thermal fluctuations due to highly ordered boundary [AOT]− bilayers templating robust near-surface layers. Exceeding the critical normal force at OCP+1.0 V causes the AFM tip to penetrate the hydrated [AOT]− layer and slide over alkyl chains, increasing friction. At OCP and OCP-1.0 V, higher friction correlates with more pronounced ripples, attributed to the rougher templating [BMIm]+ boundary layer. Kinetic experiments show that switching from OCP-1.0 V to OCP+1.0 V achieves superlubricity within 15 s, enabling real-time friction control.