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Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy
Abstract
Developing highly efficient, low-cost oxygen reduction catalysts, especially in acidic medium, is of significance toward fuel cell commercialization. Although pyrolyzed Fe-N-C catalysts have been regarded as alternatives to platinum-based catalytic materials, further improvement requires precise control of the Fe-N x structure at the molecular level and a comprehensive understanding of catalytic site structure and the ORR mechanism on these materials. In this report, we present a microporous metal–organic-framework-confined strategy toward the preferable formation of single-atom dispersed catalysts. The onset potential for Fe-N-C is 0.92 V, comparable to that of Pt/C and outperforming most noble-metal-free catalysts ever reported. A high-spin Fe 3+ -N 4 configuration is revealed by the 57 Fe Mössbauer spectrum and X-ray absorption spectroscopy for Fe L-edge, which will convert to Fe 2+ -N 4 at low potential. The in situ reduced Fe 2+ -N 4 moiety from high-spin O x -Fe 3+ -N 4 contributes to most of the ORR activity due to its high turnover frequency (TOF) of ca. 1.71 e s –1 sites –1 .
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Cites
Electrocatalyst approaches and challenges for automotive fuel cells
Debe, M. K. (2012) · Nature · doi:10.1038/nature11115 · Cited by 5,885
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
Wu, G., More, K. L., Johnston, C. M., & Zelenay, P. (2011) · Science · doi:10.1126/science.1200832 · Cited by 3,984
Atomic 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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Single atom electrocatalysts supported on graphene or graphene-like carbons
Fei, H., Dong, J., Chen, D., Hu, T., Duan, X., Shakir, I., Huang, Y., & Duan, X. (2019) · Chemical Society Reviews · doi:10.1039/c9cs00422j · Cited by 673
Recent Advances in MOF‐Derived Single Atom Catalysts for Electrochemical Applications
Song, Z., Zhang, L., Doyle‐Davis, K., Fu, X., Luo, J., & Sun, X. (2020) · Advanced Energy Materials · doi:10.1002/aenm.202001561 · Cited by 412
Ao, X., Zhang, W., Zhao, B., Ding, Y., Nam, G., Soule, L., Abdelhafiz, A., Wang, C., & Liu, M. (2020) · Energy & Environmental Science · doi:10.1039/d0ee00832j · Cited by 330
Xie, X., Shang, L., Xiong, X., Shi, R., & Zhang, T. (2022) · Advanced Energy Materials · doi:10.1002/aenm.202102688 · Cited by 291
Advances in iron-based electrocatalysts for nitrate reduction
Yuan, S., Xue, Y., Ma, R., Ma, Q., Chen, Y., & Fan, J. (2023) · Science of The Total Environment · doi:10.1016/j.scitotenv.2023.161444 · Cited by 117
Metadata
- Authors
- Xiao, M., Zhu, J., Ma, L., Jin, Z., Ge, J., Deng, X., Hou, Y., He, Q., Li, J., Jia, Q., Mukerjee, S., Yang, R., Jiang, Z., Su, D., Liu, C., & Xing, W.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-02-21
- Volume
- 8
- Issue
- 4
- Pages
- 2824-2832
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2789758237
- Cited by
- 540
- References
- 3
- FWCI
- 15.95
- Type
- journal article
- Language
- en
- Open access
- closed
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- CoChat. (2026). Citation check: Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy. https://app.cochat.ai/papers/10.1021/acscatal.8b00138
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- Xiao, M., Zhu, J., Ma, L., Jin, Z., Ge, J., Deng, X., Hou, Y., He, Q., Li, J., Jia, Q., Mukerjee, S., Yang, R., Jiang, Z., Su, D., Liu, C., & Xing, W. (2018). Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy. ACS Catalysis. https://doi.org/10.1021/acscatal.8b00138
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