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Easily Regenerated CuO/γ-Al2O3 for Persulfate-Based Catalytic Oxidation: Insights into the Deactivation and Regeneration Mechanism

  • Jun Wang
    Jun Wang
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    More by Jun Wang
  • Bin Li
    Bin Li
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    More by Bin Li
  • 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
  • Fengbao Zhang
    Fengbao Zhang
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
  • Guoliang Zhang
    Guoliang Zhang
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
  • Yuanzhi Zhu*
    Yuanzhi Zhu
    Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, China
    *Email: [email protected]
    More by Yuanzhi Zhu
  • , and 
  • Wenchao Peng*
    Wenchao Peng
    School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    *Email: [email protected]
    More by Wenchao Peng
Cite this: ACS Appl. Mater. Interfaces 2021, 13, 2, 2630–2641
Publication Date (Web):January 5, 2021
https://doi.org/10.1021/acsami.0c19013
Copyright © 2021 American Chemical Society
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Abstract

In this work, γ-Al2O3-supported CuO (c-CuO/Al2O3) materials are successfully synthesized using a novel impregnation–precipitation–decomposition method. The obtained c-CuO/Al2O3 catalyst shows excellent catalytic activities for bisphenol A (BPA) degradation with sodium persulfate (PDS) as an oxidant. Radical quenching tests and electron paramagnetic resonance (EPR) studies indicate that PDS activation is a combined mechanism involving both free radical and nonfree radical pathways. In a continuous large-scale degradation process, about 1.78 L of 20 ppm BPA can be completely removed within 480 min. Although c-CuO/Al2O3 can be deactivated after several reaction cycles, the catalytic activity can be regenerated after simple aerobic calcination. X-ray photoelectron spectroscopy (XPS) and Raman analysis confirm that the deactivation of c-CuO/Al2O3 should be attributed to the conversion of Cu(II) to Cu(I). The aerobic calcination could oxidize Cu(I) back to Cu(II), thus recovering the catalytic activity. In addition, the density functional technology (DFT) and temperature-programmed oxidation (TPD) results reveal that γ-Al2O3 can not only serve as a carrier to anchor the CuO particles but also can adsorb and activate PDS by introducing more basic sites on the surface. c-CuO/Al2O3 has high activity and can be regenerated easily, thus having great potential applications for wastewater treatment.

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This article is cited by 6 publications.

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  2. Quanbao He, Ming Ge, Qiang Yu. Synergistic degradation of tetracycline by BiOBr microspheres combined with peroxydisulfate under visible LED light irradiation. Journal of Chemical Sciences 2021, 133 (4) https://doi.org/10.1007/s12039-021-01955-w
  3. Yi Zhu, Dongya Li, Shiyu Zuo, Zeyu Guan, Su Ding, Dongsheng Xia, Xiaohu Li. Cu2O/CuO induced non-radical/radical pathway toward highly efficient peroxymonosulfate activation. Journal of Environmental Chemical Engineering 2021, 9 (6) , 106781. https://doi.org/10.1016/j.jece.2021.106781
  4. Peng Zhao, Yuwei Zhao, Yiping Guo, Rong Guo, Yimei Tian, Weigao Zhao. Preparation of CuO/γAl2O3 catalyst for degradation of azo dyes (reactive brilliant red X–3B): An optimization study. Journal of Cleaner Production 2021, 328 , 129624. https://doi.org/10.1016/j.jclepro.2021.129624
  5. Jun Wang, Bin Li, Yang Li, Xiaobin Fan, Fengbao Zhang, Guoliang Zhang, Wenchao Peng. Facile Synthesis of Atomic Fe‐N‐C Materials and Dual Roles Investigation of Fe‐N 4 Sites in Fenton‐Like Reactions. Advanced Science 2021, 8 (22) , 2101824. https://doi.org/10.1002/advs.202101824
  6. Shuaishuai Xin, Bingrui Ma, Chunlei Zhang, Xiaoming Ma, Peng Xu, Guangshan Zhang, Mengchun Gao, Yanjun Xin. Catalytic activation of peroxydisulfate by alfalfa-derived nitrogen self-doped porous carbon supported CuFeO2 for nimesulide degradation: Performance, mechanism and DFT calculation. Applied Catalysis B: Environmental 2021, 294 , 120247. https://doi.org/10.1016/j.apcatb.2021.120247