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Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction

Journal Article · · Nature Catalysis
Carbon dioxide electroreduction in aqueous media using Cu catalysts can generate many different C2 and C3 products, which leads to the question whether all products are generated from the same types of active sites or if product-specific active sites are responsible for certain products. Here, by reducing mixtures of 13CO and 12CO2, we show that oxide-derived Cu catalysts have three different types of active sites for C–C coupled products, one that produces ethanol and acetate, another that produces ethylene and yet another that produces 1-propanol. In contrast, we do not find evidence of product-specific sites on polycrystalline Cu and oriented (100) and (111) Cu surfaces. Analysis of the isotopic composition of the products leads to the prediction that the adsorption energy of *COOH (the product of the first step of CO2 reduction) may be a descriptor for the product selectivity of a given active site. Finally, these new insights should enable highly selective catalysts to be developed.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231; SC0004993
OSTI ID:
1603501
Journal Information:
Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 1 Vol. 2; ISSN 2520-1158
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (15)

In Situ Infrared Spectroscopy Reveals Persistent Alkalinity near Electrode Surfaces during CO 2 Electroreduction journal September 2019
Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design journal December 2018
A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO 2 to Value‐Added Chemicals and Fuel journal November 2019
Nitride‐Derived Copper Modified with Indium as a Selective and Highly Stable Catalyst for the Electroreduction of Carbon Dioxide journal June 2019
Two‐Dimensional Electrocatalysts for Efficient Reduction of Carbon Dioxide journal October 2019
Mechanistic reaction pathways of enhanced ethylene yields during electroreduction of CO2–CO co-feeds on Cu and Cu-tandem electrocatalysts journal October 2019
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products journal March 2019
Designing materials for electrochemical carbon dioxide recycling journal July 2019
Constraining CO coverage on copper promotes high-efficiency ethylene electroproduction journal November 2019
Selective electrochemical CO 2 conversion to multicarbon alcohols on highly efficient N-doped porous carbon-supported Cu catalysts journal January 2020
Regulating C–C coupling in thermocatalytic and electrocatalytic CO x conversion based on surface science journal January 2019
Enhanced CO 2 electroreduction performance over Cl-modified metal catalysts journal January 2019
The sensitivity of Cu for electrochemical carbon dioxide reduction to hydrocarbons as revealed by high throughput experiments journal January 2019
CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2 journal February 2020
Nitride-Derived Copper Modified with Indium as a Selective and Highly Stable Catalyst for the Electroreduction of Carbon Dioxide text January 2019

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