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Graphitic phosphorus coordinated single Fe atoms for hydrogenative transformations

Author

Listed:
  • Xiangdong Long

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Zelong Li

    (Lanzhou University)

  • Guang Gao

    (Chinese Academy of Sciences)

  • Peng Sun

    (Chinese Academy of Sciences)

  • Jia Wang

    (Chinese Academy of Sciences)

  • Bingsen Zhang

    (Chinese Academy of Sciences)

  • Jun Zhong

    (Soochow University)

  • Zheng Jiang

    (Chinese Academy of Science)

  • Fuwei Li

    (Chinese Academy of Sciences
    Dalian National Laboratory for Clean Energy)

Abstract

Single-atom metal-nitrogen-carbon (M-N-C) catalysts have sparked intensive interests, however, the development of an atomically dispersed metal-phosphorus-carbon (M-P-C) catalyst has not been achieved, although molecular metal-phosphine complexes have found tremendous applications in homogeneous catalysis. Herein, we successfully construct graphitic phosphorus species coordinated single-atom Fe on P-doped carbon, which display outstanding catalytic performance and reaction generality in the heterogeneous hydrogenation of N-heterocycles, functionalized nitroarenes, and reductive amination reactions, while the corresponding atomically dispersed Fe atoms embedded on N-doped carbon are almost inactive under the same reaction conditions. Furthermore, we find that the catalytic activity of graphitic phosphorus coordinated single-atom Fe sharply decreased when Fe atoms were transformed to Fe clusters/nanoparticles by post-impregnation Fe species. This work can be of fundamental interest for the design of single-atom catalysts by utilizing P atoms as coordination sites as well as of practical use for the application of M-P-C catalysts in heterogeneous catalysis.

Suggested Citation

  • Xiangdong Long & Zelong Li & Guang Gao & Peng Sun & Jia Wang & Bingsen Zhang & Jun Zhong & Zheng Jiang & Fuwei Li, 2020. "Graphitic phosphorus coordinated single Fe atoms for hydrogenative transformations," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17903-0
    DOI: 10.1038/s41467-020-17903-0
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    Cited by:

    1. Jiajing Pei & Huishan Shang & Junjie Mao & Zhe Chen & Rui Sui & Xuejiang Zhang & Danni Zhou & Yu Wang & Fang Zhang & Wei Zhu & Tao Wang & Wenxing Chen & Zhongbin Zhuang, 2024. "A replacement strategy for regulating local environment of single-atom Co-SxN4−x catalysts to facilitate CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Sheng Qian & Feng Xu & Yu Fan & Ningyan Cheng & Huaiguo Xue & Ye Yuan & Romain Gautier & Tengfei Jiang & Jingqi Tian, 2024. "Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Hongqiang Jin & Peipei Li & Peixin Cui & Jinan Shi & Wu Zhou & Xiaohu Yu & Weiguo Song & Changyan Cao, 2022. "Unprecedentedly high activity and selectivity for hydrogenation of nitroarenes with single atomic Co1-N3P1 sites," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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