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

Eilert, Andre; Cavalca, Filippo; Roberts, F. Sloan; Osterwalder, Jurg; Liu, Chang; Favaro, Marco; Crumlin, Ethan J.; Ogasawara, Hirohito; Friebel, Daniel; Pettersson, Lars G. M.; Nilsson, Anders

doi:10.1021/acs.jpclett.6b02273

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

Journal Article · Fri Dec 16 00:00:00 EST 2016 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.6b02273· OSTI ID:1379672

Eilert, Andre ^[1]; Cavalca, Filippo ^[1]; ^[1]; Osterwalder, Jurg ^[2]; Liu, Chang ^[3]; Favaro, Marco ^[4]; Crumlin, Ethan J. ^[4]; Ogasawara, Hirohito ^[5]; Friebel, Daniel ^[5]; Pettersson, Lars G. M. ^[3]; ^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Stockholm Univ., Stockholm (Sweden)
Univ. of Zurich, Zurich (Switzerland)
Stockholm Univ., Stockholm (Sweden)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO₂RR). 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 CO₂RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multicarbon compounds such as ethylene.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1379672

Alternate ID(s):: OSTI ID: 1361142

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 1 Vol. 8; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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