Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium
Open accessAbstract
The cathodic oxygen reduction reaction (ORR) is essential in the electrochemical energy conversion of fuel cells. Here, through the NH 3 atmosphere annealing of a graphene oxide (GO) precursor containing trace amounts of Ru, we have synthesized atomically dispersed Ru on nitrogen-doped graphene that performs as an electrocatalyst for the ORR in acidic medium. The Ru/nitrogen-doped GO catalyst exhibits excellent four-electron ORR activity, offering onset and half-wave potentials of 0.89 and 0.75 V, respectively, vs a reversible hydrogen electrode (RHE) in 0.1 M HClO 4 , together with better durability and tolerance toward methanol and carbon monoxide poisoning than seen in commercial Pt/C catalysts. X-ray adsorption fine structure analysis and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy are performed and indicate that the chemical structure of Ru is predominantly composed of isolated Ru atoms coordinated with nitrogen atoms on the graphene substrate. Furthermore, a density function theory study of the ORR mechanism suggests that a Ru-oxo-N 4 structure appears to be responsible for the ORR catalytic activity in the acidic medium. These findings provide a route for the design of efficient ORR single-atom catalysts.
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The weak pre-edge peak at 22116 eV suggests the formation of a square-pyramidal or distorted octahedral configuration.
“The pre-edge peak at 22116 eV, which is due to the 1 s to 4pz shakedown transition of a square-planar configuration, shows only a weak intensity, suggesting the formation of a square-pyramidal or distorted octahedral configuration [52].”
From Atomically dispersed ruthenium in carbon aerogels as effective catalysts for pH-universal hydrogen evolution reaction (2022) · cites this paper as [52]
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- Authors
- Zhang, C., Sha, J., Fei, H., Liu, M., Yazdi, S., Zhang, J., Zhong, Q., Zou, X., Zhao, N., Yu, H., Jiang, Z., Ringe, E., Yakobson, B. I., Dong, J., Chen, D., & Tour, J. M.
- Affiliations
- Rice University (US)
- Tianjin University (CN)
- Chinese Academy of Sciences (CN)
- Corresponding author
- Ringe, Emilie
- Yakobson, Boris I.
- Dong, Juncai
- Tour, James M.
- ORCID
- Venue
- ACS Nano
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-06-28
- Volume
- 11
- Issue
- 7
- Pages
- 6930-6941
- ISSN
- 1936-0851 (ISSN-L)
- 1936-086X
- OpenAlex
- W2726465153
- Cited by
- 545
- References
- 4
- Citations by year
- 2026: 33 · 2025: 40 · 2024: 45 · 2023: 50 · 2022: 86 · 2021: 76 · 2020: 87 · 2019: 76 · 2018: 47 · 2017: 5
- FWCI
- 15.71
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Locations
- ACS Nano (publishedVersion, other-oa)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Apollo (University of Cambridge) (submittedVersion)
- Apollo
- Funders
- Air Force Office of Scientific Research (FA9550-12-1-0035, FA9550-14-1-0111)
- Welch Foundation (C-1590)
- Basic Energy Sciences (DE-SC0012547)
- American Chemical Society Petroleum Research Fund (56256-DN15)
- National Natural Science Foundation of China (11475212, 11605225)
- China Scholarship Council (NA)
- Institute of High Energy Physics, Chinese Academy of Science (NA)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- oxygen reduction reaction, single-atom catalysts, ruthenium, nitrogen-doped graphene, graphene oxide, NH3 annealing, acidic media, four-electron pathway, ORR mechanism, fuel cell catalysts, Pt/C alternative
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