Joe Gauthier, Texas Tech University

Abstract:

Extending the reach of density functional theory: capturing charge transfer and making electrons behave

The development of an atomistic understanding of heterogeneous catalysis has transformed materials discovery: from the Edisonian approach that led to the Haber-Bosch process, to the modern physics-informed framework that allows prediction of the optimal catalyst composition before an experiment is performed. Extending this framework to interfacial charge transfer processes-such as corrosion, energy conversion and storage, electrochemical fuel synthesis—remains challenging. Experimentally, probing the electrified double layer with atomic resolution is extremely difficult, while simulations are limited by the self-interaction error (SIE) and its associated problems intrinsic to semi-local density functional theory (DFT). Most relevant to this talk is the unphysical delocalization of electron density, which results in unacceptable errors when describing ions at this level of theory. In this talk, I will share our group's efforts to overcome these challenges and extend DFT's ability to capture both charge transfer thermodynamics and kinetics. First, I will introduce a Born-Haber cycle approach for modeling corrosion thermodynamics that avoids explicit treatment of corrosion products. Using this framework, we investigated the empirically observed activity-stability tradeoff in water electrolyzer anodes and found no fundamental intrinsic coupling between these two critical parameters. I will then turn to kinetics, which requires explicit treatment of ions, and will describe our efforts to establish an experimental benchmark for evaluating density functionals in charge transfer processes. I will discuss how this benchmark informs our understanding of pH effects in hydrogen evolution electrocatalysis, and its broader implications for modeling interfacial electrochemical processes.

Bio:

Dr. Joe Gauthier is an Assistant Professor of Chemical Engineering at Texas Tech University. Dr. Gauthier graduated summa cum laude with his B.S. degree in Chemical Engineering at The Ohio State University in 2015 before moving to California to pursue doctoral research at Stanford University. After one year as a visiting student in the Physics Department at the Technical University of Denmark, he completed his PhD at Stanford in 2020. Before starting at TTU, he was a Postdoctoral Researcher at UC Berkeley and Lawrence Berkeley National Laboratory. He is the author of more than 40 peer-reviewed publications and leads a 12-person research team at TTU comprising a mix of Ph.D., M.S., and undergraduate students. At TTU, his research program focuses on heterogeneous (electro)catalysis, ultimately with the aim of solving problems related to renewable energy conversion/storage and decarbonization of the chemical industry.