Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Wang, Lei; Higgins, Drew C.; Ji, Yongfei; Morales-Guio, Carlos G.; Chan, Karen; Hahn, Christopher; Jaramillo, Thomas F.

doi:10.1073/pnas.1821683117

Title: Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Journal Article · 23 January 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1821683117 · OSTI ID:1594223

; Higgins, Drew C.; Ji, Yongfei;

;

; Hahn, Christopher; Jaramillo, Thomas F.

Electrochemical CO reduction can serve as a sequential step in the transformation of CO ₂ into multicarbon fuels and chemicals. In this study, we provide insights on how to steer selectivity for CO reduction almost exclusively toward a single multicarbon oxygenate by carefully controlling the catalyst composition and its surrounding reaction conditions. Under alkaline reaction conditions, we demonstrate that planar CuAg electrodes can reduce CO to acetaldehyde with over 50% Faradaic efficiency and over 90% selectivity on a carbon basis at a modest electrode potential of −0.536 V vs. the reversible hydrogen electrode. The Faradaic efficiency to acetaldehyde was further enhanced to 70% by increasing the roughness factor of the CuAg electrode. Density functional theory calculations indicate that Ag ad-atoms on Cu weaken the binding energy of the reduced acetaldehyde intermediate and inhibit its further reduction to ethanol, demonstrating that the improved selectivity to acetaldehyde is due to the electronic effect from Ag incorporation. These findings will aid in the design of catalysts that are able to guide complex reaction networks and achieve high selectivity for the desired product.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0004993

OSTI ID:: 1594223

Alternate ID(s):: OSTI ID: 1647600

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 23 Vol. 117; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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