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Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation
Open accessAbstract
Atomically dispersed metal-N-C structures are efficient active sites for catalyzing benzene oxidation reaction (BOR). However, the roles of N and C atoms are still unclear. We report a polymerization-regulated pyrolysis strategy for synthesizing single-atom Fe-based catalysts, and present a systematic study on the coordination effect of Fe-NxCycatalytic sites in BOR. The special coordination environment of single-atom Fe sites brings a surprising discovery: Fe atoms anchored by four-coordinating N atoms exhibit the highest BOR performance with benzene conversion of 78.4% and phenol selectivity of 100%. Upon replacing coordinated N atoms by one or two C atoms, the BOR activities decrease gradually. Theoretical calculations demonstrate the coordination pattern influences not only the structure and electronic features, but also the catalytic reaction pathway and the formation of key oxidative species. The increase of Fe-N coordination number facilitates the generation and activation of the crucial intermediate O=Fe=O species, thereby enhancing the BOR activity.
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Chen, Z., Song, Y., Cai, J., Zheng, X., Han, D., Wu, Y., Zang, Y., Niu, S., Liu, Y., Zhu, J., et al. (2018) · Angewandte Chemie International Edition · doi:10.1002/anie.201801834 · Cited by 1,075
Self-citation
Cited by
Chemical Synthesis of Single Atomic Site Catalysts
Ji, S., Chen, Y., Wang, X., Zhang, Z., Wang, D., & Li, Y. (2020) · Chemical Reviews · doi:10.1021/acs.chemrev.9b00818 · Cited by 1,444
Self-citationSingle-Atom Catalysts across the Periodic Table
Kaiser, S. K., Chen, Z., Faust Akl, D., Mitchell, S., & Pérez-Ramírez, J. (2020) · Chemical Reviews · doi:10.1021/acs.chemrev.0c00576 · Cited by 1,367
Self-citationLiu, L., & Corma, A. (2023) · Chemical Reviews · doi:10.1021/acs.chemrev.2c00733 · Cited by 689
Zhang, Y., Jiao, L., Yang, W., Xie, C., & Jiang, H. (2021) · Angewandte Chemie International Edition · doi:10.1002/anie.202016219 · Cited by 649
Xiao, X., Gao, Y., Zhang, L., Zhang, J., Zhang, Q., Li, Q., Bao, H., Zhou, J., Miao, S., Chen, N., et al. (2020) · Advanced Materials · doi:10.1002/adma.202003082 · Cited by 528
Metadata
- Authors
- Pan, Y., Chen, Y., Wu, K., Chen, Z., Liu, S., Cao, X., Cheong, W.-C., Meng, T., Luo, J., Zheng, L., Liu, C., Wang, D., Peng, Q., Li, J., & Chen, C.
- Venue
- Nature Communications
- Published
- 2019-09-19
- Volume
- 10
- Issue
- 1
- Pages
- 4290-4290
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2973980246
- Cited by
- 506
- References
- 1
- FWCI
- 20.93
- Type
- journal article
- Language
- en
- Open access
- gold
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- Pan, Y., Chen, Y., Wu, K., Chen, Z., Liu, S., Cao, X., Cheong, W.-C., Meng, T., Luo, J., Zheng, L., Liu, C., Wang, D., Peng, Q., Li, J., & Chen, C. (2019). Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation. Nature Communications. https://doi.org/10.1038/s41467-019-12362-8
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