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The Confined Interlayer Growth of Ultrathin Two-Dimensional Fe3O4 Nanosheets with Enriched Oxygen Vacancies for Peroxymonosulfate Activation

  • Weixue Wang
    Weixue Wang
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    School of Chemical Engineering, Northeast Electric Power University, Jilin 132000, P. R. China
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  • Yang Liu
    Yang Liu
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    More by Yang Liu
  • Yifan Yue
    Yifan Yue
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    More by Yifan Yue
  • Huihui Wang
    Huihui Wang
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    More by Huihui Wang
  • Gong Cheng
    Gong Cheng
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    More by Gong Cheng
  • Chunyang Gao
    Chunyang Gao
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, P. R. China
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  • Chunlin Chen
    Chunlin Chen
    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, P. R. China
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  • Yuejie Ai
    Yuejie Ai
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    More by Yuejie Ai
  • Zhe Chen*
    Zhe Chen
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    *Email: [email protected]
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  • , and 
  • Xiangke Wang
    Xiangke Wang
    MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, P. R. China
    More by Xiangke Wang
Cite this: ACS Catal. 2021, 11, 17, 11256–11265
Publication Date (Web):August 25, 2021
https://doi.org/10.1021/acscatal.1c03331
Copyright © 2021 American Chemical Society
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Abstract

Developing iron-based catalysts with superior activity and stability is a long-term goal for peroxymonosulfate (PMS) activation in advanced oxidation processes. Combining the confined interlayer growth strategy with melt infiltration under dry-chemical conditions, we successfully synthesized ultrathin 2D Fe3O4 nanosheets with a monolayer thickness of about 1 nm. Atomic force microscopy, CS-corrected high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray absorption fine structure, etc. jointly revealed that the 2D Fe3O4 nanosheets possessed special graphene-like morphology and enriched oxygen vacancies. As highly efficient AOP catalysts, a series of refractory organic pollutants, including phenolic compounds, antibiotics, and pharmaceuticals, were degraded and mineralized effectively via the activation of PMS. On the basis of radical quenching experiments, electrochemical analysis, and theory calculations, the radical generation (·OH and SO4·) and mediated electron transfer were verified to be key mechanisms in the reaction. The oxygen vacancy-rich ultrathin 2D Fe3O4 mediated the electron transfer between pollutions and oxidants, prompted the redox cycle of Fe3O4, and remarkably lowered the energy barrier for interfacial charge transfer. This work could generate 2D metal oxides nanosheets with sufficient oxygen vacancies in a large scale, leading the insight for boosting the activity of iron-based catalysts.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.1c03331.

  • Additional material synthesis, experimental procedures, electrochemical analysis tests, density functional theory calculation details and models, optimization experiments, and characterization analysis including TEM and SEM images of RUB-15 and as-prepared samples, photographs, XRD patterns, Mössbauer spectrum, low-temperature EPR spectra, zeta potential, effects of ethanol and methanol dose, six terminations along [111] direction and possible oxygen vacancies, optimized geometric structures, and tables of chemical formulas and detailed information for HPLC analysis, XPS peaks binding energies and relevant ratios, and Fenton-like catalytic performance comparison (PDF)

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