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Title: Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction

Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO 2RR). Using in situ ambient pressure X-ray photoelectron spectroscopy and quasi in situ electron energy-loss spectroscopy in a transmission electron microscope, we show that there is a substantial amount of residual oxygen in nanostructured, oxide-derived copper electrocatalysts but no residual copper oxide. On the basis of these findings in combination with density functional theory simulations, we propose that residual subsurface oxygen changes the electronic structure of the catalyst and creates sites with higher carbon monoxide binding energy. If such sites are stable under the strongly reducing conditions found in CO 2RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multicarbon compounds such as ethylene.
Authors:
 [1] ;  [1] ; ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ;  [5] ;  [3] ; ORCiD logo [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Stockholm Univ., Stockholm (Sweden)
  2. Univ. of Zurich, Zurich (Switzerland)
  3. Stockholm Univ., Stockholm (Sweden)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; In Situ; Ambient-Pressure X-Ray Photoelectron Spectroscopy; Scanning Transmission Electron Microscopy; Electron Energy Loss Spectroscopy; Density Functional Theory
OSTI Identifier:
1379672