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Title: Electroreduction of carbon monoxide over a copper nanocube catalyst: Surface structure and pH dependence on selectivity

Abstract

The activity and selectivity for CO2/CO reduction over copper electrodes is strongly dependent on the local surface structure of the catalyst and the pH of the electrolyte. Here we investigate a unique, copper nanocube surface (CuCube) as a CO reduction electrode under neutral and basic pH, using online electrochemical mass spectroscopy (OLEMS) to determine the onset potentials and relative intensities of methane and ethylene production. To relate the unique selectivity to the surface structure, the CuCube surface reactivity is compared to polycrystalline copper and three single crystals under the same reaction conditions. Here, we find that the high selectivity for ethylene over the CuCube surface is most comparable to the Cu(100) surface, which has the cubic unit cell. However, the suppression of methane production over CuCube is unique to that particular surface. Basic pH is also shown to enhance ethylene selectivity on all surfaces, again with the CuCube surface being unique.

Authors:
ORCiD logo [1];  [2];  [3]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
  2. Opus 12 Incorporated, Berkeley CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; AlbaNova University Center, Stockholm Univ., Stockholm (Sweden), Dept. of Physics
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1311816
Grant/Contract Number:  
FA9550-10-1-0572, AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 8; Journal Issue: 6; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Roberts, F. Sloan, Kuhl, Kendra P., and Nilsson, Anders. Electroreduction of carbon monoxide over a copper nanocube catalyst: Surface structure and pH dependence on selectivity. United States: N. p., 2016. Web. doi:10.1002/cctc.201501189.
Roberts, F. Sloan, Kuhl, Kendra P., & Nilsson, Anders. Electroreduction of carbon monoxide over a copper nanocube catalyst: Surface structure and pH dependence on selectivity. United States. https://doi.org/10.1002/cctc.201501189
Roberts, F. Sloan, Kuhl, Kendra P., and Nilsson, Anders. Tue . "Electroreduction of carbon monoxide over a copper nanocube catalyst: Surface structure and pH dependence on selectivity". United States. https://doi.org/10.1002/cctc.201501189. https://www.osti.gov/servlets/purl/1311816.
@article{osti_1311816,
title = {Electroreduction of carbon monoxide over a copper nanocube catalyst: Surface structure and pH dependence on selectivity},
author = {Roberts, F. Sloan and Kuhl, Kendra P. and Nilsson, Anders},
abstractNote = {The activity and selectivity for CO2/CO reduction over copper electrodes is strongly dependent on the local surface structure of the catalyst and the pH of the electrolyte. Here we investigate a unique, copper nanocube surface (CuCube) as a CO reduction electrode under neutral and basic pH, using online electrochemical mass spectroscopy (OLEMS) to determine the onset potentials and relative intensities of methane and ethylene production. To relate the unique selectivity to the surface structure, the CuCube surface reactivity is compared to polycrystalline copper and three single crystals under the same reaction conditions. Here, we find that the high selectivity for ethylene over the CuCube surface is most comparable to the Cu(100) surface, which has the cubic unit cell. However, the suppression of methane production over CuCube is unique to that particular surface. Basic pH is also shown to enhance ethylene selectivity on all surfaces, again with the CuCube surface being unique.},
doi = {10.1002/cctc.201501189},
journal = {ChemCatChem},
number = 6,
volume = 8,
place = {United States},
year = {Tue Feb 16 00:00:00 EST 2016},
month = {Tue Feb 16 00:00:00 EST 2016}
}

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