Life at constant potential: Linking theory and experiment in electrochemistry

Talk by Andrew Peterson

Associate Professor
Brown University School of Engineering


Electrochemical technologies are considered crucial to future sustainable energy scenarios. However, the complexity of these systems has hindered the first-principles understanding and design of materials for such energy conversions. In this talk, I will describe our approaches to understand electrochemical reactions based on a grand-canonical, or constant-voltage, approach to atomistic simulations, and how these calculations can be directly linked to experimental observations. I will briefly present the methodology we use, which we refer to as the "solvated jellium" approach, as well as the consistent thermodynamics which it describes. Importantly, I will discuss how we use these approaches to inform and guide experiments. First, we will show how proton transfer is coupled with (non-integer) electron transfer at the electrochemical interface - which we can relate to experiments on the measured pKa of a surface bound species. This leads to a simple Gauss Law understanding of the surface. Finally, we will link this approach to describe a fully constant-potential understanding of the hydrogen evolution reaction on platinum, and we will show that this analysis leads to a break from the conventional wisdom that the Delta G~0 hydrogens are kinetically active.


Wed 26 Feb 20


DTU Fysik


DTU Physics
Building 311
1st floor / Lounge