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Edge‐Rich Fe−N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis
Open accessAbstract
Controllably constructing nitrogen‐modified divacancies (ND) in carbon substrates to immobilize atomic Fe species and unveiling the advantageous configuration is still challenging, but indispensable for attaining optimal Fe−N−C catalysts for the oxygen reduction reaction (ORR). Herein, a fundamental investigation of unfolding intrinsically superior edge‐ND trapped atomic Fe motifs (e‐ND−Fe) relative to an intact center model (c‐ND−Fe) in ORR electrocatalysis is reported. Density functional theory calculations reveal that local electronic redistribution and bandgap shrinkage for e‐ND−Fe endow it with a lower free‐energy barrier toward direct four‐electron ORR. Inspired by this, a series of atomic Fe catalysts with adjustable ND−Fe coordination are synthesized, which verify that ORR performance highly depends on the concentration of e‐ND−Fe species. Remarkably, the best e‐ND−Fe catalyst delivers a favorable kinetic current density and halfwave potential that can be comparable to benchmark Pt−C under acidic conditions. This work will guide to develop highly active atomic metal catalysts through rational defect engineering.
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Electrocatalyst approaches and challenges for automotive fuel cells
Debe, M. K. (2012) · Nature · doi:10.1038/nature11115 · Cited by 5,885
Fei, 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
Ultralow-loading platinum-cobalt fuel cell catalysts derived from imidazolate frameworks
Chong, L., Wen, J., Kubal, J., Sen, F. G., Zou, J., Greeley, J., Chan, M., Barkholtz, H., Ding, W., & Liu, D.-J. (2018) · Science · doi:10.1126/science.aau0630 · Cited by 1,100
Self-citationHigh-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites
Zhang, H., Chung, H. T., Cullen, D. A., Wagner, S., Kramm, U. I., More, K. L., Zelenay, P., & Wu, G. (2019) · Energy & Environmental Science · doi:10.1039/c9ee00877b · Cited by 616
PGM‐Free Cathode Catalysts for PEM Fuel Cells: A Mini‐Review on Stability Challenges
Shao, Y., Dodelet, J., Wu, G., & Zelenay, P. (2019) · Advanced Materials · doi:10.1002/adma.201807615 · Cited by 553
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Advancements in cathode catalyst and cathode layer design for proton exchange membrane fuel cells
Sun, Y., Polani, S., Luo, F., Ott, S., Strasser, P., & Dionigi, F. (2021) · Nature Communications · doi:10.1038/s41467-021-25911-x · Cited by 369
A durable half-metallic diatomic catalyst for efficient oxygen reduction
Li, H., Di, S., Niu, P., Wang, S., Wang, J., & Li, L. (2022) · Energy & Environmental Science · doi:10.1039/d1ee03194e · Cited by 325
Synthesis of ultrathin porous C3N4-modified Co3O4 nanosheets for enhanced oxygen evolution reaction
Wang, H., Liu, Y., Sun, Z., Ren, J., Zou, X., & Zhang, C.-Y. (2021) · Electrochimica Acta · doi:10.1016/j.electacta.2020.137537 · Cited by 17
Metadata
- Authors
- Wang, X., Jia, Y., Mao, X., Liu, D., He, W., Li, J., Liu, J., Yan, X., Chen, J., Song, L., Du, A., & Yao, X.
- Venue
- Advanced Materials
- Publisher
- Wiley
- Published
- 2020-03-05
- Volume
- 32
- Issue
- 16
- Pages
- e2000966-e2000966
- ISSN
- 0935-9648 (ISSN-L)
- 1521-4095
- OpenAlex
- W3010225030
- Cited by
- 318
- References
- 5
- FWCI
- 10.36
- Type
- journal article
- Language
- en
- Open access
- bronze
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- Wang, X., Jia, Y., Mao, X., Liu, D., He, W., Li, J., Liu, J., Yan, X., Chen, J., Song, L., Du, A., & Yao, X. (2020). Edge‐Rich Fe−N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis. Advanced Materials. https://doi.org/10.1002/adma.202000966
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