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Regulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene

Author

Listed:
  • Ting Zhang

    (Dalian University of Technology)

  • Zhe Sun

    (Dalian University of Technology)

  • Shiyan Li

    (Chinese Academy of Science)

  • Baojun Wang

    (Taiyuan University of Technology
    Taiyuan University of Technology)

  • Yuefeng Liu

    (Chinese Academy of Science)

  • Riguang Zhang

    (Taiyuan University of Technology
    Taiyuan University of Technology)

  • Zhongkui Zhao

    (Dalian University of Technology)

Abstract

Developing highly efficient catalyst for selective oxidation of benzene to phenol (SOBP) with low H2O2 consumption is highly desirable for practical application, but challenge remains. Herein, we report unique single-atom Cu1-N1O2 coordination-structure on N/C material (Cu-N1O2 SA/CN), prepared by water molecule-mediated pre-assembly-pyrolysis method, can efficiently boost SOBP reaction at a 2:1 of low H2O2/benzene molar ratio, showing 83.7% of high benzene conversion with 98.1% of phenol selectivity. The Cu1-N1O2 sites can provide a preponderant reaction pathway for SOBP reaction with less steps and lower energy barrier. As a result, it shows an unexpectedly higher turnover frequency (435 h−1) than that of Cu1-N2 (190 h−1), Cu1-N3 (90 h−1) and Cu nanoparticle (58 h−1) catalysts, respectively. This work provides a facile and efficient method for regulating the electron configuration of single-atom catalyst and generates a highly active and selective non-precious metal catalyst for industrial production of phenol through selective oxidation of benzene.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34852-y
    DOI: 10.1038/s41467-022-34852-y
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    1. Haihong Bao & Yuan Qiu & Xianyun Peng & Jia-ao Wang & Yuying Mi & Shunzheng Zhao & Xijun Liu & Yifan Liu & Rui Cao & Longchao Zhuo & Junqiang Ren & Jiaqiang Sun & Jun Luo & Xuping Sun, 2021. "Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. 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.
    3. Yu Zhou & Zhipan Ma & Junjie Tang & Ning Yan & Yonghua Du & Shibo Xi & Kai Wang & Wei Zhang & Haimeng Wen & Jun Wang, 2018. "Immediate hydroxylation of arenes to phenols via V-containing all-silica ZSM-22 zeolite triggered non-radical mechanism," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
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