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Tailored d-Band Facilitating in Fe Gradient Doping CuO Boosts Peroxymonosulfate Activation for High Efficiency Generation and Release of Singlet Oxygen

  • Shiyu Zuo
    Shiyu Zuo
    School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, P. R. China
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  • Dongya Li*
    Dongya Li
    School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, P. R. China
    Engineering Research Center Clean Production of Textile Dyeing and Printing, Ministry of Education, Wuhan 430073, P. R. China
    *Email: [email protected]
    More by Dongya Li
  • Zeyu Guan
    Zeyu Guan
    School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, P. R. China
    More by Zeyu Guan
  • Fan Yang
    Fan Yang
    School of Electronic and Electrical Engineering, Wuhan Textile University, Wuhan 430073, P. R. China
    More by Fan Yang
  • Haiming Xu
    Haiming Xu
    School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, P. R. China
    More by Haiming Xu
  • Dongsheng Xia
    Dongsheng Xia
    School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, P. R. China
  • , and 
  • Jinquan Wan
    Jinquan Wan
    School of Environment and Energy, South China University of Technology, Guangzhou 510006, P. R. China
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Cite this: ACS Appl. Mater. Interfaces 2021, 13, 42, 49982–49992
Publication Date (Web):October 12, 2021
https://doi.org/10.1021/acsami.1c15061
Copyright © 2021 American Chemical Society
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Abstract

In the field of heterogeneous catalysis, limitations of the surface reaction process inevitably make improving the catalytic efficiency to remove pollutants in water a major challenge. Here, we report a unique structure of Fe surface-gradient-doped CuO that improves the overall catalytic processes of adsorption, electron transfer, and desorption. Interestingly, gradient doping leads to an imbalanced charge distribution in the crystal structure, thereby promoting the adsorption and electron transport efficiency of peroxymonosulfate (PMS). The orbital hybridization of Fe also improves the electronic activity. More importantly, the occupied d-orbital distribution is closer to the lower energy level, which improves the desorption of the reaction intermediate (1O2). As a result, the production and desorption of 1O2 have been improved, resulting in excellent BPA degradation ability (kinetic rate increased by 67.3 times). Two-dimensional infrared correlation spectroscopy is used to better understand the doping process and catalytic mechanism of Fe-CuO. Fe–O changes before Cu–O and is more active. The Fe-required active sites, active species intensity, and kinetic reaction rates show a good correlation. This research provides a scientific basis for expanding the purification of toxic organic pollutants in complex water environments by heterogeneous catalytic oxidation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c15061.

  • Discussions of chemicals and materials used, material characterization, electrochemical analysis tests, 2D-FTIR-COS analysis, and calculation methods, figures of line scan of Fe-CuO-3, XPS spectra, optimized structure model, DOS of CuO, degradation of BPA in different systems, adsorption of BPA, cyclic experiment, XRD pattern, XPS spectra, UPLC-MS spectrum, inhibition experiments, consumption of PMS, poisoning experiment, EPR spectrum, EIS spectra, CV curves, effects of pH, temperature, PMS concentration, Fe-CuO-3 concentration, BPA concentration, an anion, and HA concentration on the degradation and rate constants of BPA, PMS/Fe-CuO-3 degrades different contaminants, and PMS/Fe-CuO-3 treats chemical wastewater, and tables of analysis conditions for different contaminants, BET of Fe-CuO, some comparison of the catalytic performance based on nonfree radical reaction, and intermediate products measured by UPLC-MS (PDF)

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