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O2 Reduction on Graphite and Nitrogen-Doped Graphite: Experiment and Theory
Abstract
An experimental and theoretical study of electroreduction of oxygen to hydrogen peroxide is presented. The experimental measurements of nitrided Ketjenblack indicated an onset potential for reduction of approximately 0.5 V (SHE) compared to the onset potential of 0.2 V observed for untreated carbon. Quantum calculations on cluster models of nitrided and un-nitrided graphite sheets show that carbon radical sites formed adjacent to substitutional N in graphite are active for O2 electroreduction to H2O2 via and adsorbed OOH intermediate. The weak catalytic effect of untreated carbon is attributed to weaker bonding of OOH to the H atom-terminated graphite edges. Substitutional N atoms that are far from graphite sheet edges will be active, and those that are close to the edges will be less active. Interference from electrochemical reduction of H atoms on the reactive sites is considered, and it is shown that in the potential range of H2O2 formation the reactive sites are not blocked by adsorbed H atoms.
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Cited by
Metal-Free Catalysts for Oxygen Reduction Reaction
Dai, L., Xue, Y., Qu, L., Choi, H.-J., & Baek, J.-B. (2015) · Chemical Reviews · doi:10.1021/cr5003563 · Cited by 2,380
Oxygen Reduction in Alkaline Media: From Mechanisms to Recent Advances of Catalysts
Ge, X., Sumboja, A., Wuu, D., An, T., Li, B., Goh, F. W. T., Hor, T. S. A., Zong, Y., & Liu, Z. (2015) · ACS Catalysis · doi:10.1021/acscatal.5b00524 · Cited by 1,341
High oxygen-reduction activity and durability of nitrogen-doped graphene
Geng, D., Chen, Y., Chen, Y., Li, Y., Li, R., Sun, X., Ye, S., & Knights, S. (2011) · Energy & Environmental Science · doi:10.1039/c0ee00326c · Cited by 1,219
Understanding and approaches for the durability issues of Pt-based catalysts for PEM fuel cell
Shao, Y., Yin, G., & Gao, Y. (2007) · Journal of Power Sources · doi:10.1016/j.jpowsour.2007.07.004 · Cited by 1,197
Yang, S., Feng, X., Wang, X., & Müllen, K. (2011) · Angewandte Chemie International Edition · doi:10.1002/anie.201100170 · Cited by 1,109
Metadata
- Authors
- Sidik, R. A., Anderson, A. B., Subramanian, N. P., Kumaraguru, S. P., & Popov, B. N.
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 2006-01-07
- Volume
- 110
- Issue
- 4
- Pages
- 1787-1793
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2027225797
- Cited by
- 627
- References
- 0
- FWCI
- 12.02
- Type
- journal article
- Language
- en
- Open access
- closed
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- Sidik, R. A., Anderson, A. B., Subramanian, N. P., Kumaraguru, S. P., & Popov, B. N. (2006). O2 Reduction on Graphite and Nitrogen-Doped Graphite: Experiment and Theory. The Journal of Physical Chemistry B. https://doi.org/10.1021/jp055150g
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Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
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