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Novel CuCo2O4 Composite Spinel with a Meso-Macroporous Nanosheet Structure for Sulfate Radical Formation and Benzophenone-4 Degradation: Interface Reaction, Degradation Pathway, and DFT Calculation

  • Yiping Wang
    Yiping Wang
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
    More by Yiping Wang
  • Haodong Ji
    Haodong Ji
    The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, P. R. China
    More by Haodong Ji
  • Wen Liu*
    Wen Liu
    The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, P. R. China
    *E-mail: [email protected]. Tel: +86 10 62744799. Fax: +86 10 62756526.
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  • Tianshan Xue
    Tianshan Xue
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
    More by Tianshan Xue
  • Chao Liu
    Chao Liu
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
    More by Chao Liu
  • Yuting Zhang
    Yuting Zhang
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
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  • Longyan Liu
    Longyan Liu
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
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  • Qiang Wang
    Qiang Wang
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
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  • Fei Qi*
    Fei Qi
    Beijing Key Lab for Source Control Technology of Water Pollution, College of Environmental Science and Engineering, Beijing Forestry University, Beijing 100083, P. R. China
    *E-mail: [email protected], [email protected]. Tel: +86 10 62336615. Fax: +86 10 62336596.
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  • Bingbing Xu
    Bingbing Xu
    State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, P. R. China
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  • Daniel C.W. Tsang
    Daniel C.W. Tsang
    Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, P. R. China
  • , and 
  • Wei Chu
    Wei Chu
    Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, P. R. China
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Cite this: ACS Appl. Mater. Interfaces 2020, 12, 18, 20522–20535
Publication Date (Web):April 9, 2020
https://doi.org/10.1021/acsami.0c03481
Copyright © 2020 American Chemical Society
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Abstract

A series of CuCo2O4 composite spinels with an interconnected meso-macroporous nanosheet morphology were synthesized using the hydrothermal method and subsequent calcination treatment to activate peroxymonosulfate (PMS) for benzophenone-4 (BP-4) degradation. As-prepared CuCo2O4 composite spinels, especially CuCo-H3 prepared by adding cetyltrimethylammonium bromide, showed superior reactivity for PMS activation. In a typical reaction, BP-4 (10.0 mg/L) was almost completely degraded in 15 min by the activation of PMS (200.0 mg/L) using CuCo-H3 (100.0 mg/L), with only 9.2 μg/L cobalt leaching detected. Even after being used six times, the performance was not influenced by the lower leaching of ions and surface-absorbed intermediates. The possible interface mechanism of PMS activation by CuCo-H3 was proposed, wherein a unique interconnected meso-macroporous nanosheet structure, strong interactions between copper and cobalt, and cycling of Co(II)/Co(III) and Cu(I)/Cu(II) effectively facilitated PMS activation to generate SO4•– and OH, which contributed to BP-4 degradation. Furthermore, combined with intermediates detected by liquid chromatography quadrupole time-of-flight mass spectrometry and density functional theory calculation results, the degradation pathway of BP-4 involving hydroxylation and C–C bond cleavage was proposed.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c03481.

  • Texts S1–S6, including chemicals; catalyst preparation and characterization; analytical methods; effects of catalyst dosage, PMS and BP-4 concentration on BP-4 degradation and calculation of steady-state concentration of SO4•− and OH; Tables S1–S7, including comparison of reported copper-cobalt oxides with CuCo-H3; mobile phase composition and detection wavelength; name, synthesis method, CTAB amounts, specific surface area, average pore diameter, and pore volume of as-prepared CuCo2O4; wt % of O, Co, and Cu; comparison of cobalt leaching; water quality parameters of secondary effluent; and identified intermediates of BP-4 degradation; and Figures S1–S15, including SEM images of CuCo-H5 and CuCo-H10; influence of borate buffer solution; cobalt ion leaching; the performance of different CuCo2O4 composite spinels; reuse of CuCo-H3; Effects of catalyst dosage, PMS and BP-4 concentration on BP-4 degradation; pH changes during reaction; determination of pHpzc value of CuCo-H3; effect of ionic strength; the contribution of Cu2+ to BP-4 degradation; XRD patterns of fresh and used CuCo-H3; effects of Cl, HCO3 and H2PO4 on BP-4 degradation; degradation of BA and NB by PMS oxidation; Cu LMM Auger spectra; and mass spectra of BP-4 degradation intermediates (PDF)

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