Trends in Oxygenate/hydrocarbon Selectivity for Electrochemical CO Reduction to C Products

Overview

Journal Nat Commun

Specialty Biology

Date 2022 Mar 18

PMID 35302055

Authors

Hong-Jie Peng

Michael T Tang

Joakim Halldin Stenlid

Xinyan Liu

Frank Abild-Pedersen

Affiliations

Soon will be listed here.

Abstract

The electrochemical conversion of carbon di-/monoxide into commodity chemicals paves a way towards a sustainable society but it also presents one of the great challenges in catalysis. Herein, we present the trends in selectivity towards specific dicarbon oxygenate/hydrocarbon products from carbon monoxide reduction on transition metal catalysts, with special focus on copper. We unveil the distinctive role of electrolyte pH in tuning the dicarbon oxygenate/hydrocarbon selectivity. The understanding is based on density functional theory calculated energetics and microkinetic modeling. We identify the critical reaction steps determining selectivity and relate their transition state energies to two simple descriptors, the carbon and hydroxide binding strengths. The atomistic insight gained enables us to rationalize a number of experimental observations and provides avenues towards the design of selective electrocatalysts for liquid fuel production from carbon di-/monoxide.

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