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Identification of the Highly Active Co–N4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide
Open accessAbstract
High Resolution Image Download MS PowerPoint Slide Electrosynthesis of hydrogen peroxide (H 2 O 2 ) through oxygen reduction reaction (ORR) is an environment-friendly and sustainable route for obtaining a fundamental product in the chemical industry. Co–N 4 single-atom catalysts (SAC) have sparkled attention for being highly active in both 2e – ORR, leading to H 2 O 2 and 4e – ORR, in which H 2 O is the main product. However, there is still a lack of fundamental insights into the structure–function relationship between CoN 4 and the ORR mechanism over this family of catalysts. Here, by combining theoretical simulation and experiments, we unveil that pyrrole-type CoN 4 (Co–N SAC Dp ) is mainly responsible for the 2e – ORR, while pyridine-type CoN 4 catalyzes the 4e – ORR. Indeed, Co–N SAC Dp exhibits a remarkable H 2 O 2 selectivity of 94% and a superb H 2 O 2 yield of 2032 mg for 90 h in a flow cell, outperforming most reported catalysts in acid media. Theoretical analysis and experimental investigations confirm that Co–N SAC Dp ─with weakening O 2 /HOO* interaction─boosts the H 2 O 2 production.
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Cites
Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction
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Enabling direct H2O2 production through rational electrocatalyst design
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Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H2O2 production
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Self-citationPolymer-Derived Heteroatom-Doped Porous Carbon Materials
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Self-citationTuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
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Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination
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Cited by
Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)
Song, W., Xiao, C., Ding, J., Huang, Z., Yang, X., Zhang, T., Mitlin, D., & Hu, W. (2024) · Advanced Materials · doi:10.1002/adma.202301477 · Cited by 373
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Balamurugan, J., Austeria, P. M., Kim, J. B., Jeong, E., Huang, H., Kim, D. H., Koratkar, N., & Kim, S. O. (2023) · Advanced Materials · doi:10.1002/adma.202302625 · Cited by 281
Metadata
- Authors
- Chen, S., Luo, T., Li, X., Chen, K., Fu, J., Liu, K., Cai, C., Wang, Q., Li, H., Chen, Y., Ma, C., Zhu, L., Lu, Y.-R., Chan, T.-S., Zhu, M., Cortés, E., & Liu, M.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2022-08-03
- Volume
- 144
- Issue
- 32
- Pages
- 14505-14516
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W4289711467
- Cited by
- 560
- References
- 62
- FWCI
- 19.76
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Chen, S., Luo, T., Li, X., Chen, K., Fu, J., Liu, K., Cai, C., Wang, Q., Li, H., Chen, Y., Ma, C., Zhu, L., Lu, Y.-R., Chan, T.-S., Zhu, M., Cortés, E., & Liu, M. (2022). Identification of the Highly Active Co–N4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.2c01194
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