Theoretical Investigation of the Adsorbate and Potential‐Induced Stability of Cu Facets During Electrochemical CO2 and CO Reduction

Author:

Yu Henry12ORCID,Govindarajan Nitish12ORCID,Weitzner Stephen E.12ORCID,Serra‐Maia Rui F.3ORCID,Akhade Sneha A.12ORCID,Varley Joel B.12ORCID

Affiliation:

1. Materials Science Division Lawrence Livermore National Laboratory Livermore CA 94550 USA

2. Laboratory for Energy Applications for the Future Lawrence Livermore National Laboratory Livermore CA 94550 USA

3. Department of Materials Science and Engineering University of Pennsylvania Philadelphia PA 19104 USA

Abstract

AbstractThe activity and product selectivity of electrocatalysts for reactions like the carbon dioxide reduction reaction (CO2RR) are intimately dependent on the catalyst's structure and composition. While engineering catalytic surfaces can improve performance, discovering the key sets of rational design principles remains challenging due to limitations in modeling catalyst stability under operating conditions. Herein, we perform first‐principles density functional calculations adopting implicit solvation methods with potential control to study the influence of adsorbates and applied potential on the stability of different facets of model Cu electrocatalysts. Using coverage dependencies extracted from microkinetic models, we describe an approach for calculating potential and adsorbate‐dependent contributions to surface energies under reaction conditions, where Wulff constructions are used to understand the morphological evolution of Cu electrocatalysts under CO2RR conditions. We identify that CO*, a key reaction intermediate, exhibits higher kinetically and thermodynamically accessible coverages on (100) relative to (111) facets, which can translate into an increased relative stabilization of the (100) facet during CO2RR. Our results support the known tendency for increased (111) faceting of Cu nanoparticles under more reducing conditions and that the relative increase in (100) faceting observed under CO2RR conditions is likely attributed to differences in CO* coverage between these facets.

Funder

Advanced Manufacturing Office

Publisher

Wiley

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