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Title: Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy

Abstract

Nanostructured copper cathodes are among the most efficient and selective catalysts to date for making multicarbon products from the electrochemical carbon dioxide reduction reaction (CO2RR). We report an in situ X-ray absorption spectroscopy investigation of the formation of a copper nanocube CO2RR catalyst with high activity that highly favors ethylene over methane production. The results show that the precursor for the copper nanocube formation is copper(I)-oxide, not copper(I)-chloride as previously assumed. A second route to an electrochemically similar material via a copper(II)–carbonate/hydroxide is also reported. In conclusion, this study highlights the importance of using oxidized copper precursors for constructing selective CO2 reduction catalysts and shows the precursor oxidation state does not affect the electrocatalyst selectivity toward ethylene formation.

Authors:
 [1];  [1];  [1];  [2]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis, Dept. of Chemical Engineering; Stockholm Univ. (Sweden). AlbaNova University Center, Dept. of Physics
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1256341
Grant/Contract Number:  
FA9550-10-1-0572; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 7; Journal Issue: 8; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Eilert, André, Roberts, F. Sloan, Friebel, Daniel, and Nilsson, Anders. Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy. United States: N. p., 2016. Web. doi:10.1021/acs.jpclett.6b00367.
Eilert, André, Roberts, F. Sloan, Friebel, Daniel, & Nilsson, Anders. Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy. United States. doi:10.1021/acs.jpclett.6b00367.
Eilert, André, Roberts, F. Sloan, Friebel, Daniel, and Nilsson, Anders. Mon . "Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy". United States. doi:10.1021/acs.jpclett.6b00367. https://www.osti.gov/servlets/purl/1256341.
@article{osti_1256341,
title = {Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy},
author = {Eilert, André and Roberts, F. Sloan and Friebel, Daniel and Nilsson, Anders},
abstractNote = {Nanostructured copper cathodes are among the most efficient and selective catalysts to date for making multicarbon products from the electrochemical carbon dioxide reduction reaction (CO2RR). We report an in situ X-ray absorption spectroscopy investigation of the formation of a copper nanocube CO2RR catalyst with high activity that highly favors ethylene over methane production. The results show that the precursor for the copper nanocube formation is copper(I)-oxide, not copper(I)-chloride as previously assumed. A second route to an electrochemically similar material via a copper(II)–carbonate/hydroxide is also reported. In conclusion, this study highlights the importance of using oxidized copper precursors for constructing selective CO2 reduction catalysts and shows the precursor oxidation state does not affect the electrocatalyst selectivity toward ethylene formation.},
doi = {10.1021/acs.jpclett.6b00367},
journal = {Journal of Physical Chemistry Letters},
number = 8,
volume = 7,
place = {United States},
year = {2016},
month = {4}
}

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