Dissolution patterns of gold on various structural surfaces in thiosulfate solutions: The effect of interface adsorption on thiosulfate oxidation and gold atom dissociation

Abstract

Passivation caused by the adsorption and decomposition of thiosulfate on gold surfaces significantly influences the leaching rate of gold. The surface structure often determines the reactivity of an interface. Studying the effects of different surfaces on the decomposition of thiosulfate ions and gold dissolution can provide insights into the passivation formation mechanism. In this study, the oxidation of thiosulfate on different surfaces is investigated using linear voltammetry. The oxidation response of thiosulfate was weaker on granular (1 1 1) and (5 4 1) surfaces than on nanoflakes with (1 1 1) surface. Furthermore, the Tafel test results indicate that the potential for gold dissolution is higher on the granular (1 1 1) and (5 4 1) surfaces, leading to a smaller current value of gold dissolution. Raman spectroscopy indicates that the response signals of the polysulfides and polythionate were stronger on the granular (1 1 1) and (5 4 1) surfaces. The chemical bond changes of thiosulfate adsorbed on different surfaces are studied through molecular simulations based on density functional theory. These results indicate that as the saturation of surface gold atoms decreases, their reaction activity increases, and the bonding effect with thiosulfate ions becomes stronger during adsorption. The changes in the SS bonds in thiosulfate reflect the influence of the different surfaces on their stability. On the (1 1 1) surface, the SS bond changes from the initial 2.102 Å to the adsorbed 2.254 Å, while on the (5 4 1) surface, the SS bond changes to 2.274 Å Although the reaction activity of the granular (1 1 1) and (5 4 1) surfaces is high, the energy barrier for dissociating individual gold atoms from them is higher. The adsorption of sulfur-containing substances on the surface, along with the increased energy barrier for gold dissociation are both factor contributing to the greater difficulty of gold dissolution from granular (1 1 1) and (5 4 1) surfaces.