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High-rate electroreduction of carbon monoxide to multi-carbon products

Journal Article · · Nature Catalysis
Carbon monoxide electrolysis has previously been reported to yield enhanced multi-carbon (C2+) Faradaic efficiencies of up 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 C18O reduction experiments suggest that the enhanced activity is due to a higher surface pH under CO reduction conditions, which facilitates the production of acetate. Here, at optimal operating conditions, we achieve a C2+ Faradaic efficiency of ~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.
Research Organization:
Univ. of Delaware, Newark, DE (United States)
Sponsoring Organization:
USDOE Office of Fossil Energy (FE)
Grant/Contract Number:
FE0029868; AC02-06CH11357
OSTI ID:
1712666
Alternate ID(s):
OSTI ID: 1614347
Journal Information:
Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 10 Vol. 1; ISSN 2520-1158
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (26)

Shape-Controlled CO 2 Electrochemical Reduction on Nanosized Pd Hydride Cubes and Octahedra journal January 2019
Bipyridine‐Assisted Assembly of Au Nanoparticles on Cu Nanowires To Enhance the Electrochemical Reduction of CO 2 journal August 2019
Highly Selective Production of Ethylene by the Electroreduction of Carbon Monoxide journal December 2019
Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper journal March 2020
Titelbild: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. 11/2020) journal March 2020
Bipyridine-Assisted Assembly of Au Nanoparticles on Cu Nanowires To Enhance the Electrochemical Reduction of CO 2 journal August 2019
Highly Selective Production of Ethylene by the Electroreduction of Carbon Monoxide journal December 2019
Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper journal January 2020
Cover Picture: Hydroxide Is Not a Promoter of C 2+ Product Formation in the Electrochemical Reduction of CO on Copper (Angew. Chem. Int. Ed. 11/2020) journal January 2020
Structure‐Sensitivity and Electrolyte Effects in CO 2 Electroreduction: From Model Studies to Applications journal June 2019
Electrochemical Carbon Dioxide Splitting journal February 2019
Efficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites journal November 2019
Formation of carbon–nitrogen bonds in carbon monoxide electrolysis journal August 2019
Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper journal February 2019
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products journal March 2019
Perfluorocarbon nanoemulsion promotes the delivery of reducing equivalents for electricity-driven microbial CO2 reduction journal April 2019
Two-dimensional copper nanosheets for electrochemical reduction of carbon monoxide to acetate journal April 2019
Designing materials for electrochemical carbon dioxide recycling journal July 2019
Constraining CO coverage on copper promotes high-efficiency ethylene electroproduction journal November 2019
Carbon monoxide electroreduction as an emerging platform for carbon utilization journal December 2019
Frustrated Lewis pairs photocatalyst for visible light-driven reduction of CO to multi-carbon chemicals journal January 2019
Improving selectivity of CO reduction via reducing the coordination of critical intermediates journal January 2019
Advances and challenges in electrochemical CO 2 reduction processes: an engineering and design perspective looking beyond new catalyst materials journal January 2020
CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2 journal February 2020
Sputtered Platinum Thin-films for Oxygen Reduction in Gas Diffusion Electrodes: A Model System for Studies under Realistic Reaction Conditions journal April 2019
Sputtered Platinum Thin-films for Oxygen Reduction in Gas Diffusion Electrodes: A Model System for Studies under Realistic Reaction Conditions text January 2019

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