Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction
Open accessAbstract
Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO 2 RR). 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 2 RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multicarbon compounds such as ethylene.
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The concentration of CO2 dissolved in the electrolyte in H cells is 34 mM at room temperature.
“In H cells the current density is limited (typically under 100 mA/cm 2 ) by the available CO2 dissolved in the electrolyte, which is only 34 mM at room temperature.[121]”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [121]
In H cells, the current density is limited (typically under 100 mA/cm2) by the available CO2 dissolved in the electrolyte.
“In H cells the current density is limited (typically under 100 mA/cm 2 ) by the available CO2 dissolved in the electrolyte, which is only 34 mM at room temperature.[121]”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [121]
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- Authors
- Eilert, A., Cavalca, F., Roberts, F. S., Osterwalder, J., Liu, C., Favaro, M., Crumlin, E. J., Ogasawara, H., Friebel, D., Pettersson, L. G. M., & Nilsson, A.
- Affiliations
- Stockholm University (SE)
- University of Zurich (CH)
- Lawrence Berkeley National Laboratory (US)
- SLAC National Accelerator Laboratory (US)
- Corresponding author
- Nilsson, Anders
- ORCID
- Venue
- The Journal of Physical Chemistry Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-12-21
- Volume
- 8
- Issue
- 1
- Pages
- 285-290
- ISSN
- 1948-7185 (ISSN-L)
- OpenAlex
- W2565135807
- Cited by
- 443
- References
- 46
- Citations by year
- 2026: 26 · 2025: 33 · 2024: 50 · 2023: 45 · 2022: 50 · 2021: 62 · 2020: 59 · 2019: 51 · 2018: 43 · 2017: 24
- FWCI
- 10.68
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Locations
- The Journal of Physical Chemistry Letters (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- eScholarship (California Digital Library) (submittedVersion)
- Funders
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
- Basic Energy Sciences (DE-SC0004993)
- Air Force Office of Scientific Research (FA9550-10-1-0572)
- Stanford University
- Stanford Institute for Materials and Energy Sciences, Stanford University
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
- Keywords
- oxide-derived copper, carbon dioxide reduction, subsurface oxygen, residual oxygen, copper electrocatalysts, electronic structure, ethylene production, multi-carbon products
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