Transforming CO2 into Sulfur-Doped Carbon As a High-Efficiency Persulfate Catalyst for the Degradation of 2,4-Dichlorphenol: Influential Factors, Activation Mechanism, and Regeneration of Catalyst

  • Yongsong Ma
    Yongsong Ma
    Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, School of Resource and Environmental Science, Wuhan University, Wuhan 430072, China
    More by Yongsong Ma
  • Yuxing Gu
    Yuxing Gu
    Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, School of Resource and Environmental Science, Wuhan University, Wuhan 430072, China
    More by Yuxing Gu
  • Da Jiang
    Da Jiang
    Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, School of Resource and Environmental Science, Wuhan University, Wuhan 430072, China
    More by Da Jiang
  • Xuhui Mao
    Xuhui Mao
    Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, School of Resource and Environmental Science, Wuhan University, Wuhan 430072, China
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  • , and 
  • Dihua Wang*
    Dihua Wang
    Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, School of Resource and Environmental Science, Wuhan University, Wuhan 430072, China
    State Key Laboratory of Water Resources and Hydropower Engineering Science, Wuhan University, Wuhan 430072, China
    *Tel.: +86-27-68774216. Email: [email protected]
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Cite this: ACS EST Water 2021, 1, 8, 1796–1806
Publication Date (Web):July 21, 2021
https://doi.org/10.1021/acsestwater.1c00112
Copyright © 2021 American Chemical Society
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Abstract

The burning of fossil fuels leads to the emission of large amounts of CO2 into the air, and how to deal with the increasingly generated CO2 has been a great challenge. In an effort to convert the low-value CO2 into valuable material, this work proposed sulfur-doped CO2 converted carbon (S-EC) by molten salt carbon capture electrochemical transformation (MSCC-ET) as a persulfate (PS) activator for 2,4-dichlorophenol (2,4-DCP) removal. The catalytic performance of CO2 converted carbon (EC) was dramatically enhanced by sulfur modification. The most efficient dosage of S-EC was 50 mg L–1; the most efficient dosage of PS was 5:1 M for PS/2,4-DCP, and the efficient pH range was 3.0–9.0. The results of radical quenching experiments and electron paramagnetic resonance spectroscopy further confirmed the novel nonradical process in a S-EC/PS system. Furthermore, the novel nonradical activation mechanism of S-EC on PS was further identified on the basis of the results of density functional theory (DFT) calculations and polarization curves. In addition, the degradation intermediates such as 4-chlorophenol, 2-chlorophenol, 2-chlorohydroquinone, and some carboxylic acids were identified by gas chromatography–mass spectrometry (GC–MS), and the possible degradation pathways were summarized. Remarkably, the molten salt redox-sulfidation method can completely restore the catalytic performance of used S-EC for PS. This work extends the application of EC materials for environmental remediation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsestwater.1c00112.

  • Discussions of high-performance liquid chromatography analysis, electron paramagnetic resonance (EPR) test, GC–MS analysis, electrochemical analysis tests, and theoretical calculation methods, figures of relevant thermodynamic calculations, detected intermediates by GC–MS, residual PS after experiment, consumption of PS, ζ potentials, EPR spectra, and illustration of the number of atoms, and tables of removal rate comparison, Fukui indices for electrophilic attack, relevant calculation results, and Mulliken atomic charges of PS adsorption (PDF)

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