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O: Fachverband Oberflächenphysik

O 47: Metal Substrates I

O 47.1: Vortrag

Mittwoch, 20. März 2024, 10:30–10:45, MA 043

Studying facet-selective adsorption of CO on Cu using the random phase approximation — •Seungchang Han and Stefan Ringe — Department of Chemistry, Korea University

Electrochemical CO2 reduction is a promising sustainable strategy for producing valuable chemicals and fuels. Cu is the only catalyst that produces significant amounts of higher reduced products like ethylene, ethanol, or methane. The product selectivity depends critically on the Cu active site environment, defined by the coverage and distribution of the central *CO intermediate. Unfortunately, one of the most successful approaches to studying adsorption events, the Perdew-Burke-Ernzerhof (PBE) functional based on generalized gradient approximation (GGA), has been shown to benefit from error compensation, which can affect their transferability to unknown systems. It also leads to a wrong prediction of adsorption trends across different surface facets and adsorption sites. Adding many-body corrections based on the random phase approximation (RPA) has been shown to critically improve the prediction of adsorption energies and long-range interactions. In this work, we first present a simple extrapolation scheme to overcome the difficulty of getting converged RPA-based adsorption energies. We then demonstrate the first trends of adsorption energies as well as the coverage dependence and compare them to conventional functionals.

Keywords: Electrochemical CO2 reduction reaction; Adsorption; Energy; Density functional theory; Random phase approximation