Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis

  • Xuning Li
    Xuning Li
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
    More by Xuning Li
  • Xiang Huang
    Xiang Huang
    Department of Physics, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
    More by Xiang Huang
  • Shibo Xi
    Shibo Xi
    Institute of Chemical and Engineering Sciences, A*STAR, 1 Pesek Road, Singapore 627833, Singapore
    More by Shibo Xi
  • Shu Miao
    Shu Miao
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    More by Shu Miao
  • Jie Ding
    Jie Ding
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    More by Jie Ding
  • Weizheng Cai
    Weizheng Cai
    School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
    More by Weizheng Cai
  • Song Liu
    Song Liu
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
    University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
    More by Song Liu
  • Xiaoli Yang
    Xiaoli Yang
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
    More by Xiaoli Yang
  • Hongbin Yang
    Hongbin Yang
    School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
    More by Hongbin Yang
  • Jiajian Gao
    Jiajian Gao
    School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
    More by Jiajian Gao
  • Junhu Wang
    Junhu Wang
    State Key Laboratory of Catalysis,  Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    More by Junhu Wang
  • Yanqiang Huang*
    Yanqiang Huang
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    *[email protected]
  • Tao Zhang
    Tao Zhang
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People’s Republic of China
    University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
    More by Tao Zhang
  • , and 
  • Bin Liu*
    Bin Liu
    School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
    *[email protected]
    More by Bin Liu
Cite this: J. Am. Chem. Soc. 2018, 140, 39, 12469–12475
Publication Date (Web):August 30, 2018
https://doi.org/10.1021/jacs.8b05992
Copyright © 2018 American Chemical Society
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Abstract

The Fenton-like process presents one of the most promising strategies to generate reactive oxygen-containing radicals to deal with the ever-growing environmental pollution. However, developing improved catalysts with adequate activity and stability is still a long-term goal for practical application. Herein, we demonstrate single cobalt atoms anchored on porous N-doped graphene with dual reaction sites as highly reactive and stable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS). Our experiments and density functional theory (DFT) calculations show that the CoN4 site with a single Co atom serves as the active site with optimal binding energy for PMS activation, while the adjacent pyrrolic N site adsorbs organic molecules. The dual reaction sites greatly reduce the migration distance of the active singlet oxygen produced from PMS activation and thus improve the Fenton-like catalytic performance.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b05992.

  • Characterization and catalytic performance of materials, simulation details, Figures S1–S23, Tables S1–S6, and notes S1 and S2 (PDF)

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