The DOI matches its Crossref record; 9 of the 9 references it cites were found in a registry or an index.
Tuning the Coordination Environment in Single-Atom Catalysts to Achieve Highly Efficient Oxygen Reduction Reactions
Abstract
Designing atomically dispersed metal catalysts for oxygen reduction reaction (ORR) is a promising approach to achieve efficient energy conversion. Herein, we develop a template-assisted method to synthesize a series of single metal atoms anchored on porous N,S-codoped carbon (NSC) matrix as highly efficient ORR catalysts to investigate the correlation between the structure and their catalytic performance. The structure analysis indicates that an identical synthesis method results in distinguished structural differences between Fe-centered single-atom catalyst (Fe-SAs/NSC) and Co-centered/Ni-centered single-atom catalysts (Co-SAs/NSC and Ni-SAs/NSC) because of the different trends of each metal ion in forming a complex with the N,S-containing precursor during the initial synthesis process. The Fe-SAs/NSC mainly consists of a well-dispersed FeN 4 S 2 center site where S atoms form bonds with the N atoms. The S atoms in Co-SAs/NSC and Ni-SAs/NSC, on the other hand, form metal–S bonds, resulting in CoN 3 S 1 and NiN 3 S 1 center sites. Density functional theory (DFT) reveals that the FeN 4 S 2 center site is more active than the CoN 3 S 1 and NiN 3 S 1 sites, due to the higher charge density, lower energy barriers of the intermediates, and products involved. The experimental results indicate that all three single-atom catalysts could contribute high ORR electrochemical performances, while Fe-SAs/NSC exhibits the highest of all, which is even better than commercial Pt/C. Furthermore, Fe-SAs/NSC also displays high methanol tolerance as compared to commercial Pt/C and high stability up to 5000 cycles. This work provides insights into the rational design of the definitive structure of single-atom catalysts with tunable electrocatalytic activities for efficient energy conversion.
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Cites
Design of electrocatalysts for oxygen- and hydrogen-involving energy conversion reactions
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Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces
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Self-citationAtomically dispersed Ni(i) as the active site for electrochemical CO2 reduction
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Self-citationFei, H., Dong, J., Feng, Y., Allen, C. S., Wan, C., Volosskiy, B., Li, M., Zhao, Z., Wang, Y., Sun, H., et al. (2018) · Nature Catalysis · doi:10.1038/s41929-017-0008-y · Cited by 1,973
Self-citationAtomic cobalt on nitrogen-doped graphene for hydrogen generation
Fei, H., Dong, J., Arellano-Jiménez, M. J., Ye, G., Dong Kim, N., Samuel, E. L. G., Peng, Z., Zhu, Z., Qin, F., Bao, J., et al. (2015) · Nature Communications · doi:10.1038/ncomms9668 · Cited by 1,621
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Molecular metal–Nx centres in porous carbon for electrocatalytic hydrogen evolution
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Self-citationZhang, H., An, P., Zhou, W., Guan, B. Y., Zhang, P., Dong, J., & Lou, X. W. (. (2018) · Science Advances · doi:10.1126/sciadv.aao6657 · Cited by 584
Cited by
Shi, Y., Ma, Z.-R., Xiao, Y.-Y., Yin, Y.-C., Huang, W.-M., Huang, Z.-C., Zheng, Y.-Z., Mu, F.-Y., Huang, R., Shi, G.-Y., et al. (2021) · Nature Communications · doi:10.1038/s41467-021-23306-6 · Cited by 894
Peng, L., Yang, J., Yang, Y., Qian, F., Wang, Q., Sun‐Waterhouse, D., Shang, L., Zhang, T., & Waterhouse, G. I. N. (2022) · Advanced Materials · doi:10.1002/adma.202202544 · Cited by 478
Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts
Wan, W., Zhao, Y., Wei, S., Triana, C. A., Li, J., Arcifa, A., Allen, C. S., Cao, R., & Patzke, G. R. (2021) · Nature Communications · doi:10.1038/s41467-021-25811-0 · Cited by 432
Self-citationElectrocatalysis of Single-Atom Sites: Impacts of Atomic Coordination
Lu, B., Liu, Q., & Chen, S. (2020) · ACS Catalysis · doi:10.1021/acscatal.0c01950 · Cited by 394
Liu, M., Li, N., Cao, S., Wang, X., Lu, X., Kong, L., Xu, Y., & Bu, X. (2022) · Advanced Materials · doi:10.1002/adma.202107421 · Cited by 341
Metadata
- Authors
- Zhang, J., Zhao, Y., Chen, C., Huang, Y.-C., Dong, C.-L., Chen, C.-J., Liu, R.-S., Wang, C., Yan, K., Li, Y., & Wang, G.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-12-05
- Volume
- 141
- Issue
- 51
- Pages
- 20118-20126
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2993510745
- Cited by
- 989
- References
- 9
- FWCI
- 23.14
- Type
- journal article
- Language
- en
- Open access
- closed
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