A Surface Reconstruction Route to High Productivity and Selectivity in CO2 Electroreduction toward C2+ Hydrocarbons

Md Golam Kibria; Cao-Thang Dinh; Ali Seifitokaldani; Phil De Luna; Thomas Burdyny; Rafael Quintero-Bermudez; Michael B Ross; Oleksandr S Bushuyev; F Pelayo García de Arquer; Peidong Yang; David Sinton; Edward H Sargent

doi:10.1002/adma.201804867

A Surface Reconstruction Route to High Productivity and Selectivity in CO₂ Electroreduction toward C₂₊ Hydrocarbons

Adv Mater. 2018 Dec;30(49):e1804867. doi: 10.1002/adma.201804867. Epub 2018 Oct 9.

Authors

Md Golam Kibria¹, Cao-Thang Dinh¹, Ali Seifitokaldani¹, Phil De Luna², Thomas Burdyny³, Rafael Quintero-Bermudez¹, Michael B Ross^{4

5}, Oleksandr S Bushuyev¹, F Pelayo García de Arquer¹, Peidong Yang^{4

5

6

7

8

9}, David Sinton³, Edward H Sargent¹

Affiliations

¹ Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, ON, M5S 3G4, Canada.
² Department of Materials Science and Engineering, University of Toronto, Toronto, ON, Canada 184 College St, Toronto, ON, M5S 3E4, Canada.
³ Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, ON, M5S 3G8, Canada.
⁴ Bio-inspired Solar Energy Program, Canadian Institute for Advanced Research, Toronto, Ontario, M5G 1Z8, Canada.
⁵ Department of Chemistry, University of California, Berkeley, Berkeley, CA, 94720, USA.
⁶ Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, CA, 94720, USA.
⁷ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁸ Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁹ Kavli Energy Nanosciences Institute, University of California, Berkeley, Berkeley, CA, 94720, USA.

PMID: 30302836
DOI: 10.1002/adma.201804867

Abstract

Electrochemical carbon dioxide reduction (CO₂ ) is a promising technology to use renewable electricity to convert CO₂ into valuable carbon-based products. For commercial-scale applications, however, the productivity and selectivity toward multi-carbon products must be enhanced. A facile surface reconstruction approach that enables tuning of CO₂ -reduction selectivity toward C₂₊ products on a copper-chloride (CuCl)-derived catalyst is reported here. Using a novel wet-oxidation process, both the oxidation state and morphology of Cu surface are controlled, providing uniformity of the electrode morphology and abundant surface active sites. The Cu surface is partially oxidized to form an initial Cu (I) chloride layer which is subsequently converted to a Cu (I) oxide surface. High C₂₊ selectivity on these catalysts are demonstrated in an H-cell configuration, in which 73% Faradaic efficiency (FE) for C₂₊ products is reached with 56% FE for ethylene (C₂ H₄ ) and overall current density of 17 mA cm^-2 . Thereafter, the method into a flow-cell configuration is translated, which allows operation in a highly alkaline medium for complete suppression of CH₄ production. A record C₂₊ FE of ≈84% and a half-cell power conversion efficiency of 50% at a partial current density of 336 mA cm^-2 using the reconstructed Cu catalyst are reported.

Keywords: CO2 electroreduction; Cu-based catalysts; flow-cells; hydrocarbons.

Abstract

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