Quantum–continuum simulation of underpotential deposition at electrified metal–solution interfaces

Abstract

Thin films: How to overachieve at underpotentials The deposition of atomically thin metal films can be predicted with a comprehensive model incorporating realistic environmental factors. Nanomaterials used as catalysts and sensors are often produced by the spontaneous attachment of metal ions onto inert metal surfaces in the underpotential regime, where the depositing metal would normally dissolve in the surrounding liquid environment. Stephen Weitzner and Ismaila Dabo from the Pennsylvania State University have developed a procedure to resolve the perplexing inability of quantum-mechanical simulations to estimate the stability of underpotential deposits, such as copper ions onto gold surfaces. The researchers used a quantum–continuum approach to account for solvent effects and Monte Carlo simulations to understand how electrification of the gold–water interface impacts deposition. These computations revealed the need to include the interfacial charge and co-adsorbed ions to accurately simulate underpotential deposition.