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Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation

Author

Listed:
  • Yuan Pan

    (Tsinghua University
    China University of Petroleum (East China))

  • Yinjuan Chen

    (Tsinghua University
    China University of Petroleum (East China))

  • Konglin Wu

    (Tsinghua University
    Anhui Normal University)

  • Zheng Chen

    (Tsinghua University)

  • Shoujie Liu

    (Tsinghua University
    Anhui Normal University)

  • Xing Cao

    (Tsinghua University)

  • Weng-Chon Cheong

    (Tsinghua University)

  • Tao Meng

    (Beijing Institute of Technology)

  • Jun Luo

    (Tianjin University of Technology)

  • Lirong Zheng

    (Chinese Academy of Sciences)

  • Chenguang Liu

    (China University of Petroleum (East China))

  • Dingsheng Wang

    (Tsinghua University)

  • Qing Peng

    (Tsinghua University)

  • Jun Li

    (Tsinghua University)

  • Chen Chen

    (Tsinghua University)

Abstract

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-NxCy catalytic 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.

Suggested Citation

  • Yuan Pan & Yinjuan Chen & Konglin Wu & Zheng Chen & Shoujie Liu & Xing Cao & Weng-Chon Cheong & Tao Meng & Jun Luo & Lirong Zheng & Chenguang Liu & Dingsheng Wang & Qing Peng & Jun Li & Chen Chen, 2019. "Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12362-8
    DOI: 10.1038/s41467-019-12362-8
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    Cited by:

    1. Jijia Xie & Xiyi Li & Jian Guo & Lei Luo & Juan J. Delgado & Natalia Martsinovich & Junwang Tang, 2023. "Highly selective oxidation of benzene to phenol with air at room temperature promoted by water," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Wei Tan & Shaohua Xie & Duy Le & Weijian Diao & Meiyu Wang & Ke-Bin Low & Dave Austin & Sampyo Hong & Fei Gao & Lin Dong & Lu Ma & Steven N. Ehrlich & Talat S. Rahman & Fudong Liu, 2022. "Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity," Nature Communications, Nature, vol. 13(1), pages 1-16, December.
    3. Jiabin Wu & Xianyu Zhu & Qun Li & Qiang Fu & Bingxue Wang & Beibei Li & Shanshan Wang & Qingchao Chang & Huandong Xiang & Chengliang Ye & Qiqiang Li & Liang Huang & Yan Liang & Dingsheng Wang & Yulian, 2024. "Enhancing radiation-resistance and peroxidase-like activity of single-atom copper nanozyme via local coordination manipulation," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    4. Deyou Yu & Licong Xu & Kaixing Fu & Xia Liu & Shanli Wang & Minghua Wu & Wangyang Lu & Chunyu Lv & Jinming Luo, 2024. "Electronic structure modulation of iron sites with fluorine coordination enables ultra-effective H2O2 activation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    5. Shuo Zhang & Jianghua Wu & Mengting Zheng & Xin Jin & Zihan Shen & Zhonghua Li & Yanjun Wang & Quan Wang & Xuebin Wang & Hui Wei & Jiangwei Zhang & Peng Wang & Shanqing Zhang & Liyan Yu & Lifeng Dong , 2023. "Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. 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.
    7. Kangkang Sun & Hongbin Shan & Helfried Neumann & Guo-Ping Lu & Matthias Beller, 2022. "Efficient iron single-atom catalysts for selective ammoxidation of alcohols to nitriles," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    8. Siliu Lyu & Chenxi Guo & Jianing Wang & Zhongjian Li & Bin Yang & Lecheng Lei & Liping Wang & Jianping Xiao & Tao Zhang & Yang Hou, 2022. "Exceptional catalytic activity of oxygen evolution reaction via two-dimensional graphene multilayer confined metal-organic frameworks," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    9. Dong Cao & Haoxiang Xu & Hongliang Li & Chen Feng & Jie Zeng & Daojian Cheng, 2022. "Volcano-type relationship between oxidation states and catalytic activity of single-atom catalysts towards hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    10. Chao-Hai Gu & Song Wang & Ai-Yong Zhang & Chang Liu & Jun Jiang & Han-Qing Yu, 2024. "Tuning electronic structure of metal-free dual-site catalyst enables exclusive singlet oxygen production and in-situ utilization," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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