Electrochemical CO2 Reduction: Classifying Cu Facets

TY - JOUR

T1 - Electrochemical CO2 Reduction: Classifying Cu Facets

AU - Bagger, Alexander

AU - Ju, Wen

AU - Sofia Varela, Ana

AU - Strasser, Peter

AU - Rossmeisl, Jan

PY - 2019/9/6

Y1 - 2019/9/6

N2 - For CO2 reduction reactions, the Cu catalyst is unique, as compared with other metals, because of its ability to produce a wide range of hydrocarbon and oxygenated products. Previously, we have shown that Cu has the unique property of binding CO∗ without having H∗ UPD (underpotential deposited). However, the product distribution from Cu depends highly on the exact nature of the Cu surface. In this work, we investigate a series of Cu facets to understand how they affect the product distribution. Some carbon-carbon (CC)-coupled products are statistically shown to highly correlate, while other CC products correlate with C1 products. We avoid studying the complex reaction network of the CO2 reduction reaction and focus instead on descriptors for the Cu facet product distribution. The coordination number distribution and the binding energies of the intermediates calculated by density functional theory are investigated as descriptors. The binding energies are close for the Cu facets, and the variation shows that two noncorrelating (orthogonal) binding energies contain up to 70% of the information from the binding energies. Further, structural analysis allows us to uniquely identify the (100)×(110) step sites as specific ethanol-producing sites from the CO2 reduction reaction.

AB - For CO2 reduction reactions, the Cu catalyst is unique, as compared with other metals, because of its ability to produce a wide range of hydrocarbon and oxygenated products. Previously, we have shown that Cu has the unique property of binding CO∗ without having H∗ UPD (underpotential deposited). However, the product distribution from Cu depends highly on the exact nature of the Cu surface. In this work, we investigate a series of Cu facets to understand how they affect the product distribution. Some carbon-carbon (CC)-coupled products are statistically shown to highly correlate, while other CC products correlate with C1 products. We avoid studying the complex reaction network of the CO2 reduction reaction and focus instead on descriptors for the Cu facet product distribution. The coordination number distribution and the binding energies of the intermediates calculated by density functional theory are investigated as descriptors. The binding energies are close for the Cu facets, and the variation shows that two noncorrelating (orthogonal) binding energies contain up to 70% of the information from the binding energies. Further, structural analysis allows us to uniquely identify the (100)×(110) step sites as specific ethanol-producing sites from the CO2 reduction reaction.

KW - CO2 reduction

KW - copper

KW - facets

KW - electrochemistry

KW - CO reduction

U2 - 10.1021/acscatal.9b01899

DO - 10.1021/acscatal.9b01899

M3 - Journal article

SN - 2155-5435

VL - 9

SP - 7894

EP - 7899

JO - ACS Catalysis

JF - ACS Catalysis

IS - 9

ER -