Journal
NATURE CATALYSIS
Volume 1, Issue 10, Pages 748-755Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-018-0133-2
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Funding
- Department of Energy [DE-FE0029868]
- National Science Foundation Faculty Early Career Development Program [CBET-1350911]
- Department of Energy Office of Science [DE-AC02-06CH11357]
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Carbon monoxide electrolysis has previously been reported to yield enhanced multi-carbon (C2+) Faradaic efficiencies of up to similar to 55%, but only at low reaction rates. This is due to the low solubility of CO in aqueous electrolytes and operation in batch-type reactors. Here, we present a high-performance CO flow electrolyser with a well controlled electrode-electrolyte interface that can reach total current densities of up to 1 A cm(-2), together with improved C2+ selectivities. Computational transport modelling and isotopic (CO)-O-18 reduction experiments suggest that the enhanced activity is due to a higher surface pH under CO reduction conditions, which facilitates the production of acetate. At optimal operating conditions, we achieve a C2+ Faradaic efficiency of similar to 91% with a C2+ partial current density over 630 mA cm(-2). Further investigations show that maintaining an efficient triple-phase boundary at the electrode-electrolyte interface is the most critical challenge in achieving a stable CO/CO2 electrolysis process at high rates.
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