Highly selective and productive reduction of carbon dioxide to multicarbon products via in situ CO management using segmented tandem electrodes

Zhang, Tianyu; Bui, Justin C.; Li, Zhengyuan; Bell, Alexis T.; Weber, Adam Z.; Wu, Jingjie

doi:10.1038/s41929-022-00751-0

Highly selective and productive reduction of carbon dioxide to multicarbon products via in situ CO management using segmented tandem electrodes

Journal Article · Wed Mar 02 23:00:00 EST 2022 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-022-00751-0· OSTI ID:1867397

Zhang, Tianyu ^[1]; ^[2]; Li, Zhengyuan ^[1]; ^[3]; ^[4]; ^[1]

Univ. of Cincinnati, OH (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Electrochemical CO₂ reduction provides a promising route to the sustainable generation of valuable chemicals and fuels. Tandem catalysts enable sequential CO₂-to-CO and CO-to-multicarbon (C₂₊) product conversions on complementary active sites, to produce high C₂₊ Faradaic efficiency (FE). Unfortunately, previous tandem catalysts exhibit poor management of CO intermediates, which diminishes C₂₊ FE. Here, we design segmented gas-diffusion electrodes (s-GDEs) in which a CO-selective catalyst layer (CL) segment at the inlet prolongs CO residence time in the subsequent C₂₊-selective segment, enhancing conversion. This phenomenon enables increases in both the CO utilization and C₂₊ current density for a Cu/Ag s-GDE compared to pure Cu, by increasing the *CO coverage within the Cu CL. Lastly, we develop a Cu/Fe-N-C s-GDE with 90% C₂₊ FE at C₂₊ partial current density (j_C2+) exceeding 1 A cm^-2. These results prove the importance of transport and establish design principles to improve C₂₊ FE and j_C2+ in tandem CO₂ reduction.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE); National Institutes of Health; National Science Foundation (NSF); National Science Foundation Graduate Research Fellowship; Army Research Office (ARO)

Grant/Contract Number:: AC02-05CH11231; FE0031919; SC0004993

OSTI ID:: 1867397

Alternate ID(s):: OSTI ID: 1867886
OSTI ID: 2478519

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 3 Vol. 5; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Highly selective and productive reduction of carbon dioxide to multicarbon products via in situ CO management using segmented tandem electrodes

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