Constant-potential reactions at the electrochemical interface
Andrew Peterson a
a Brown University, Hope Street, 184, Providence, United States
Proceedings of International Conference on Electrocatalysis for Energy Applications and Sustainable Chemicals (EcoCat)
Online, Spain, 2020 November 23rd - 25th
Organizers: Ward van der Stam, Marta Costa Figueiredo, Sixto Gimenez Julia, Núria López and Bastian Mei
Invited Speaker, Andrew Peterson, presentation 029
Publication date: 6th November 2020

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. I'll 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 cover the methodology we have developed, which we refer to as the "solvated jellium" approach, which enables electronically grand-canonical calculations to run at comparable cost to canonical calculations. A key ramification of processes at constant potential is that the number of electrons involved in a reaction is not known a priori, and is not in general an integer quantity. Examples will be provided on how we use these approaches to inform and guide experiments.

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