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Fine-Tuning Radical/Nonradical Pathways on Graphene by Porous Engineering and Doping Strategies

  • Xintong Li
    Xintong Li
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    Department of Chemistry, City University of Hong Kong, Kowloon 999077, Hong Kong
    More by Xintong Li
  • Jun Wang
    Jun Wang
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    More by Jun Wang
  • Xiaoguang Duan*
    Xiaoguang Duan
    School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide South Australia 5005, Australia
    *Email: [email protected] adelaide.edu.au
  • Yang Li
    Yang Li
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    More by Yang Li
  • Xiaobin Fan
    Xiaobin Fan
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    More by Xiaobin Fan
  • Guoliang Zhang
    Guoliang Zhang
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
  • Fengbao Zhang
    Fengbao Zhang
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
  • , and 
  • Wenchao Peng*
    Wenchao Peng
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    *Email: [email protected]. Tel.: 86-22-85356119.
    More by Wenchao Peng
Cite this: ACS Catal. 2021, 11, 8, 4848–4861
Publication Date (Web):April 6, 2021
https://doi.org/10.1021/acscatal.0c05089
Copyright © 2021 American Chemical Society
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Abstract

Nitrogen and sulfur co-doped graphene (N,S-G) is activated using ZnCl2, KOH, and CO2 to develop different defects and functionalities. The modified carbo-catalysts are used to activate peroxymonosulfate (PMS) for phenol degradation. Compared with nitrogen-doped graphene (N-G), N,S-G exhibits better catalytic activity, and KOH activation further enhances the oxidation efficiency. Radical quenching experiments, electrochemical characterization, and electron paramagnetic resonance characterization reveal that N-G activates PMS via a nonradical pathway. The involvement of a secondary sulfur dopant will transform the reaction pathway into radical-dominated oxidation (SO4•–and OH). KOH activation further promotes the generation of the two radical species and further involves superoxide ion radicals (O2•–), thus achieving deeper mineralization of the organic pollutants. Different from the nonradical species confined on the catalyst surface, radical oxidation (including the singlet oxygen (1O2) transformed from O2•–) occurs in bulk solution and protects the carbo-catalyst from corrosion, herein securing better structural integrity and stability of carbo-catalysts. Based on the structure–activity features, we designed a high-performance scalable carbo-catalyst of KOH-activated and N,S-codoped graphene (N,S-G-rGO-KOH) using a facile strategy, which is promising for practical applications.

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