Incorporation of Nitrogen Defects for Efficient Reduction of CO2 via Two-Electron Pathway on Three-Dimensional Graphene Foam
Abstract
The practical recycling of carbon dioxide (CO2) by the electrochemical reduction route requires an active, stable, and affordable catalyst system. Although noble metals such as gold and silver have been demonstrated to reduce CO2 into carbon monoxide (CO) efficiently, they suffer from poor durability and scarcity. Here we report three-dimensional (3D) graphene foam incorporated with nitrogen defects as a metal-free catalyst for CO2 reduction. The nitrogen-doped 3D graphene foam requires negligible onset overpotential (-0.19 V) for CO formation, and it exhibits superior activity over Au and Ag, achieving similar maximum Faradaic efficiency for CO production (∼85%) at a lower overpotential (-0.47 V) and better stability for at least 5 h. The dependence of catalytic activity on N-defect structures is unraveled by systematic experimental investigations. Indeed, the density functional theory calculations confirm pyridinic N as the most active site for CO2 reduction, consistent with experimental results.
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In contrast, other groups have reported that Cu+ is rapidly reduced and remains as Cu0 under reducing conditions.
“In contrast to the above reports on the crucial role of Cu + , other groups have reported that Cu + is rapidly reduced and remains as Cu 0 under reducing conditions.[103]”
From Electrochemical CO <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [103]
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 <sub>2</sub> Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [103]
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- Authors
- Wu, J., Liu, M., Sharma, P. P., Yadav, R. M., Ma, L., Yang, Y., Zou, X., Zhou, X.-D., Vajtai, R., Yakobson, B. I., Lou, J., & Ajayan, P. M.
- Affiliations
- Rice University (US)
- University of South Carolina (US)
- Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States
- Corresponding author
- Yakobson, Boris I.
- Lou, Jun
- Ajayan, Pulickel M.
- ORCID
- Venue
- Nano Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-12-11
- Volume
- 16
- Issue
- 1
- Pages
- 466-470
- ISSN
- 1530-6984 (ISSN-L)
- 1530-6992
- OpenAlex
- W2199531033
- Cited by
- 520
- References
- 27
- Citations by year
- 2026: 22 · 2025: 36 · 2024: 36 · 2023: 36 · 2022: 60 · 2021: 72 · 2020: 67 · 2019: 87 · 2018: 62 · 2017: 29 · 2016: 13
- FWCI
- 10.27
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Nano Letters (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Welch Foundation (C-1716)
- Air Force Office of Scientific Research (FA9550-12-1-0035)
- 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 › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
- Keywords
- CO2 reduction, electrochemical CO2 reduction, nitrogen defects, metal-free catalysts, two-electron pathway, carbon monoxide production, pyridinic nitrogen, Faradaic efficiency, catalyst stability
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