TY - JOUR

T1 - Theoretical Optimization of Compositions of High-Entropy Oxides for the Oxygen Evolution Reaction**

AU - Svane, Katrine L.

AU - Rossmeisl, Jan

N1 - Funding Information: This work is supported by the Danish National Research Foundation Center for High‐Entropy Alloy Catalysis (CHEAC) DNRF‐149. Publisher Copyright: © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

PY - 2022

Y1 - 2022

N2 - High-entropy oxides are oxides consisting of five or more metals incorporated in a single lattice, and the large composition space suggests that properties of interest can be readily optimised. For applications within catalysis, the different local atomic environments result in a distribution of binding energies for the catalytic intermediates. Using the oxygen evolution reaction on the rutile (110) surface as example, here we outline a strategy for the theoretical optimization of the composition. Density functional theory calculations performed for a limited number of sites are used to fit a model that predicts the reaction energies for all possible local atomic environments. Two reaction pathways are considered; the conventional pathway on the coordinatively unsaturated sites and an alternative pathway involving transfer of protons to a bridging oxygen. An explicit model of the surface is constructed to describe the interdependency of the two pathways and identify the composition that maximizes catalytic activity.

AB - High-entropy oxides are oxides consisting of five or more metals incorporated in a single lattice, and the large composition space suggests that properties of interest can be readily optimised. For applications within catalysis, the different local atomic environments result in a distribution of binding energies for the catalytic intermediates. Using the oxygen evolution reaction on the rutile (110) surface as example, here we outline a strategy for the theoretical optimization of the composition. Density functional theory calculations performed for a limited number of sites are used to fit a model that predicts the reaction energies for all possible local atomic environments. Two reaction pathways are considered; the conventional pathway on the coordinatively unsaturated sites and an alternative pathway involving transfer of protons to a bridging oxygen. An explicit model of the surface is constructed to describe the interdependency of the two pathways and identify the composition that maximizes catalytic activity.

KW - Density Functional Calculations

KW - Electrochemistry

KW - High-Entropy Oxides

KW - Oxygen Evolution Reaction

U2 - 10.1002/anie.202201146

DO - 10.1002/anie.202201146

M3 - Journal article

C2 - 35225378

AN - SCOPUS:85126043945

VL - 61

JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

SN - 1433-7851

IS - 19

M1 - e202201146

ER -