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A cocoon silk chemistry strategy to ultrathin N-doped carbon nanosheet with metal single-site catalysts

Author

Listed:
  • Youqi Zhu

    (Tsinghua University)

  • Wenming Sun

    (China Building Materials Academy)

  • Jun Luo

    (Tianjin University of Technology)

  • Wenxing Chen

    (Tsinghua University)

  • Tai Cao

    (Tsinghua University)

  • Lirong Zheng

    (Chinese Academy of Sciences)

  • Juncai Dong

    (Chinese Academy of Sciences)

  • Jian Zhang

    (Tsinghua University)

  • Maolin Zhang

    (Tsinghua University)

  • Yunhu Han

    (Tsinghua University)

  • Chen Chen

    (Tsinghua University)

  • Qing Peng

    (Tsinghua University)

  • Dingsheng Wang

    (Tsinghua University)

  • Yadong Li

    (Tsinghua University)

Abstract

Development of single-site catalysts supported by ultrathin two-dimensional (2D) porous matrix with ultrahigh surface area is highly desired but also challenging. Here we report a cocoon silk chemistry strategy to synthesize isolated metal single-site catalysts embedded in ultrathin 2D porous N-doped carbon nanosheets (M-ISA/CNS, M = Fe, Co, Ni). X-ray absorption fine structure analysis and spherical aberration correction electron microscopy demonstrate an atomic dispersion of metal atoms on N-doped carbon matrix. In particular, the Co-ISA/CNS exhibit ultrahigh specific surface area (2105 m2 g−1) and high activity for C–H bond activation in the direct catalytic oxidation of benzene to phenol with hydrogen peroxide at room temperature, while the Co species in the form of phthalocyanine and metal nanoparticle show a negligible activity. Density functional theory calculations discover that the generated O = Co = O center intermediates on the single Co sites are responsible for the high activity of benzene oxidation to phenol.

Suggested Citation

  • Youqi Zhu & Wenming Sun & Jun Luo & Wenxing Chen & Tai Cao & Lirong Zheng & Juncai Dong & Jian Zhang & Maolin Zhang & Yunhu Han & Chen Chen & Qing Peng & Dingsheng Wang & Yadong Li, 2018. "A cocoon silk chemistry strategy to ultrathin N-doped carbon nanosheet with metal single-site catalysts," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-06296-w
    DOI: 10.1038/s41467-018-06296-w
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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. Qichen Wang & Qingguo Feng & Yongpeng Lei & Shuaihao Tang & Liang Xu & Yu Xiong & Guozhao Fang & Yuchao Wang & Peiyao Yang & Jingjing Liu & Wei Liu & Xiang Xiong, 2022. "Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Ting Zhang & Zhe Sun & Shiyan Li & Baojun Wang & Yuefeng Liu & Riguang Zhang & Zhongkui Zhao, 2022. "Regulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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