Frequency Dependent Silica Dissolution Rate Enhancement under Oscillating Pressure via an Electrochemical Pressure Solution-like, Surface Resonance Mechanism

From atomic force microscopy (AFM) experiments, we report a new phenomenon in which the dissolution rate of fused silica is enhanced by more than 5 orders of magnitude by simply pressing a second, dissimilar surface against it and oscillating the contact pressure at low kHz frequencies in deionized water. The silica dissolution rate enhancement was found to exhibit a strong dependence on the pressure oscillation frequency consistent with a resonance effect. This harmonic enhancement of the silica dissolution rate was only observed at asymmetric material interfaces (e.g., diamond on silica) with no evidence of dissolution rate enhancement observed at symmetric material interfaces (i.e., silica on silica) within the experimental time scales. The apparent requirement for interface dissimilarity, the results of analogous experiments performed in anhydrous dodecane, and the observation that the silica dissolution pits continue to grow in size under contact stresses well below the silica yield stress refute a mechanical deformation or chemo-mechanical origin to the observed phenomenon. Instead, the silica dissolution rate enhancement exhibits characteristics consistent with a previously described `electrochemical pressure solution' mechanism, albeit, with greatly amplified kinetics. Using a framework of electrochemical pressure solution, an electrochemical model of mineral dissolution, and a recently proposed surface resonance theory, we present an electrochemo-mechanical mechanism that explains how oscillating the contact pressure between dissimilar surfaces in water can amplify surface dissolution rates by many orders of magnitude. This reaction rate enhancement mechanism has implications not only for dissolution but also for potentially other reactions occurring at the solid-liquid interface, e.g. catalysis.

Automated summary

In this study, a new phenomenon of enhancing the dissolution rate of fused silica was discovered by conducting atomic force microscopy experiments. By pressing a second, dissimilar surface against the silica and oscillating the contact pressure in deionized water, the dissolution rate was enhanced by more than 5 orders of magnitude. This enhancement was only observed at asymmetric material interfaces and exhibited characteristics consistent with the electrochemical pressure solution mechanism.