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

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1603501
Grant/Contract Number:  
AC02-05CH11231; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalytic mechanisms; electrocatalysis; energy; heterogeneous catalysis

Citation Formats

Lum, Yanwei, and Ager, Joel W. Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction. United States: N. p., 2018. Web. doi:10.1038/s41929-018-0201-7.
Lum, Yanwei, & Ager, Joel W. Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction. United States. https://doi.org/10.1038/s41929-018-0201-7
Lum, Yanwei, and Ager, Joel W. Mon . "Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction". United States. https://doi.org/10.1038/s41929-018-0201-7. https://www.osti.gov/servlets/purl/1603501.
@article{osti_1603501,
title = {Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction},
author = {Lum, Yanwei and Ager, Joel W.},
abstractNote = {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.},
doi = {10.1038/s41929-018-0201-7},
journal = {Nature Catalysis},
number = 1,
volume = 2,
place = {United States},
year = {Mon Dec 17 00:00:00 EST 2018},
month = {Mon Dec 17 00:00:00 EST 2018}
}

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