Adsorbate-Driven Electrode Processes, Part 1: Faceting and Anisotropic Dissolution

Abstract

Monolayers of adsorbates on metal surfaces under electrochemical conditions can promote faceting of the underlying electrode surfaces, and facilitate anisotropic dissolution. Here we use density functional theory (DFT) to model these metal-adsorbate interactions. We train Behler-Parrinello neural networks to approximate the DFT potential energy surfaces of stepped surfaces. We use these neural networks to identify adsorbate structures near step edges and demonstrate that the long-range order of the adsorbate adlattice drives anisotropic dissolution.