CO 2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu 2 O Films

Li, Christina W.; Kanan, Matthew W.

doi:10.1021/ja3010978

Cited by 2,000CO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionCatalysts for Methane Reforming

CO 2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu 2 O Films

Li, Christina W., Kanan, Matthew W.·2012·Journal of the American Chemical Society

DOI 10.1021/ja3010978

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Abstract

Modified Cu electrodes were prepared by annealing Cu foil in air and electrochemically reducing the resulting Cu(2)O layers. The CO(2) reduction activities of these electrodes exhibited a strong dependence on the initial thickness of the Cu(2)O layer. Thin Cu(2)O layers formed by annealing at 130 °C resulted in electrodes whose activities were indistinguishable from those of polycrystalline Cu. In contrast, Cu(2)O layers formed at 500 °C that were ≥~3 μm thick resulted in electrodes that exhibited large roughness factors and required 0.5 V less overpotential than polycrystalline Cu to reduce CO(2) at a higher rate than H(2)O. The combination of these features resulted in CO(2) reduction geometric current densities >1 mA/cm(2) at overpotentials <0.4 V, a higher level of activity than all previously reported metal electrodes evaluated under comparable conditions. Moreover, the activity of the modified electrodes was stable over the course of several hours, whereas a polycrystalline Cu electrode exhibited deactivation within 1 h under identical conditions. The electrodes described here may be particularly useful for elucidating the structural properties of Cu that determine the distribution between CO(2) and H(2)O reduction and provide a promising lead for the development of practical catalysts for electrolytic fuel synthesis.

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Mandal et al. did not detect CO2RR products as long as Cu2O was present at the catalyst surface.
“For example, using surface sensitive in-situ Raman spectroscopy with selected-ion flow tube mass spectrometry, Mandal et al. did not detect CO2RR products as long as Cu2O was present at the catalyst surface (Figure.7).[104]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [104]
Their DFT studies suggested that the reduction of Cu2O is favored both kinetically and energetically over CO2RR.
“Their DFT studies suggested that the reduction of Cu2O is favored both kinetically and energetically over CO2RR.”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [104]
In contrast, a few other DFT studies reveal that sub-surface oxygen has negligible effect on the CO2RR activity of Cu.
“In contrast to the above reports, a few other DFT studies reveal that sub-surface oxygen has negligible effect on the CO2RR activity of Cu. [103,104]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [104]

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Authors: Li, C. W., & Kanan, M. W.
Affiliations: Stanford University (US)
Corresponding author: Kanan, Matthew W.
ORCID: Li, Christina W.
Kanan, Matthew W.
Venue: Journal of the American Chemical Society
Publisher: American Chemical Society (ACS)
Published: 2012-04-20
Volume: 134
Issue: 17
Pages: 7231-7234
ISSN: 0002-7863 (ISSN-L)
1520-5126
DOI: 10.1021/ja3010978
OpenAlex: W2082498048
Cited by: 2,000
References: 29
Citations by year: 2026: 84 · 2025: 109 · 2024: 126 · 2023: 128 · 2022: 168 · 2021: 189 · 2020: 235 · 2019: 194 · 2018: 210 · 2017: 181 · 2016: 155 · 2015: 105 · 2014: 64 · 2013: 44 · 2012: 8
FWCI: 27.14
Type: journal article
Language: en
Open access: closed
Locations: Journal of the American Chemical Society (publishedVersion)
PubMed (publishedVersion)
Funders: National Science Foundation
Stanford Precourt Institute for Energy
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: CO2 reduction, copper electrode, low overpotential, electrode surface roughness, film thickness dependence, annealing temperature, electrode deactivation, electrocatalysis

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CO 2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu 2 O Films

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