Insights into the Oxygen Evolution Reaction on Graphene-Based Single-Atom Catalysts from First-Principles-Informed Microkinetic Modeling
At a Glance
Section titled âAt a Glanceâ| Metadata | Details |
|---|---|
| Publication Date | 2023-03-31 |
| Journal | ACS Catalysis |
| Authors | Michael Rebarchik, Saurabh Bhandari, Thomas Kropp, Manos Mavrikakis |
| Institutions | University of WisconsinâMadison, UniversitĂ© Bourgogne Franche-ComtĂ© |
| Citations | 30 |
Abstract
Section titled âAbstractâSingle-atom transition metals embedded in nitrogen-doped graphene have emerged as promising electrocatalysts due to their high activity and low material cost. These materials have been shown to catalyze a variety of electrochemical reactions, but their active sites under reaction conditions remain poorly understood. Using first-principles density functional theory calculations, we develop a pH-dependent microkinetic model to evaluate the relative performance of transition metal catalysts embedded in fourfold N-substituted double carbon vacancies in graphene for the oxygen evolution reaction. We find that reaction pathways involving intermediates co-adsorbed on the metal site are preferred on all transition metals. These pathways lead to enhancements in catalytic activity and broaden the activity peak when compared with purely thermodynamics-based predictions. Furthermore, these findings demonstrate the importance of investigating reaction pathways on graphene-based catalysts and other two-dimensional (2D) materials that involve metal active centers decorated by spectator intermediate species.