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Origin of the Enhanced Reusability and Electron Transfer of the Carbon-Coated Mn3O4 Nanocube for Persulfate Activation

  • Yani Liu
    Yani Liu
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China
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  • Jun Luo
    Jun Luo
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China
    More by Jun Luo
  • Lin Tang*
    Lin Tang
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China
    *Email: [email protected]. Phone: +86-731-88822778. Fax: +86-731-88823701.
    More by Lin Tang
  • Chengyang Feng
    Chengyang Feng
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China
  • Jiajia Wang
    Jiajia Wang
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China
    More by Jiajia Wang
  • Yaocheng Deng
    Yaocheng Deng
    College of Resources and Environment, Hunan Agricultural University, Changsha 410082, China
  • Haoyu Liu
    Haoyu Liu
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    More by Haoyu Liu
  • Jiangfang Yu
    Jiangfang Yu
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
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  • Haopeng Feng
    Haopeng Feng
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
    More by Haopeng Feng
  • , and 
  • Jingjing Wang
    Jingjing Wang
    College of Environmental Science and Engineering, Hunan University, Changsha 410082, China
Cite this: ACS Catal. 2020, 10, 24, 14857–14870
Publication Date (Web):December 3, 2020
https://doi.org/10.1021/acscatal.0c04049
Copyright © 2020 American Chemical Society
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Abstract

Manganese oxides and carbon materials are both desirable catalysts for persulfate (PS) advanced oxidation processes in environmental remediation. Nevertheless, manganese oxides suffer from low reusability while carbon materials face the problem of limited catalytic efficiency. For the purpose of making full use of the advantages of the two materials as well as avoiding their shortcomings, carbon-coated Mn3O4 composites (Mn3O4/C) with a regular nanocube structure were designed to activate PS for the removal of organics, and the catalytic processes were deeply investigated. The catalyst prepared at 400 °C with a precursor ratio (glucose/KMnO4) of 0.5 exhibited the best catalytic performance along with satisfactory reusability owing to the protection of the outer carbon layer. According to experimental results and density functional theory calculation, there were van der Waals interaction and a part of the strong attraction between the interface of PS and Mn3O4/C, which could be enhanced by inner Mn3O4 and thus promoted the electron transfer between PS and carbon shell, and the defective edges of the carbon layer with hydroxyl (C–OH) groups could act as active sites for PS activation. Radical (SO4•–, OH) and nonradical (1O2) oxidation processes both participated in the degradation of 2,4-dichlorophenol, in which OH was dominating. This study not only proposed a promising catalyst for the degradation of pollutants but also expanded research ideas for future PS activation mechanism studies by integrating the experiment and simulation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.0c04049.

  • Experimental detection method and pseudo-first-order kinetics fitting model; XRD, SEM, nitrogen adsorption–desorption isotherms, FTIR spectrum, and XPS survey of the catalyst; TOC changes of 2,4-D; pseudo first-order kinetics fitting of the reaction; effects of PS and catalyst dosage; zeta potentials of 0.5-Mn3O4/C-T4; linear correlation results between pH and kobs; dynamic changes of solution pH with the low PS concentration; molecular structure of pollutants; degradation of 2,4-D by different carbon materials; cyclic voltammograms; optimized structures of models for DFT calculation; RDG isosurfaces of COH/PS; effects of MeOH and TBA on 2,4-D removal efficiency; decomposition of PS in the presence of NaN3; pore structure parameters of materials; and distance, bond length, and Bader charge in different structures (PDF)

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  2. Jie Miao, Yuan Zhu, Junyu Lang, Jingzhen Zhang, Shixian Cheng, Baoxue Zhou, Lizhi Zhang, Pedro J. J. Alvarez, Mingce Long. Spin-State-Dependent Peroxymonosulfate Activation of Single-Atom M–N Moieties via a Radical-Free Pathway. ACS Catalysis 2021, 11 (15) , 9569-9577. https://doi.org/10.1021/acscatal.1c02031
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  27. Yangju Li, Haoran Dong, Long Li, Junyang Xiao, Shuangjie Xiao, Zilan Jin. Efficient degradation of sulfamethazine via activation of percarbonate by chalcopyrite. Water Research 2021, 202 , 117451. https://doi.org/10.1016/j.watres.2021.117451
  28. Lei Dong, Xiong Pan, Sheng Zhang, Li Lin, Guochuan Yin. Research Progress on degradation of Organic pollutants in Water Body by Iron-based Materials activated persulfate. Journal of Physics: Conference Series 2021, 2009 (1) , 012035. https://doi.org/10.1088/1742-6596/2009/1/012035
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