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Efficient Removal of Organic Pollutants by Metal–organic Framework Derived Co/C Yolk–Shell Nanoreactors: Size-Exclusion and Confinement Effect

  • Ming Zhang
    Ming Zhang
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Ming Zhang
  • Chengming Xiao
    Chengming Xiao
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
  • Xin Yan
    Xin Yan
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Xin Yan
  • Saisai Chen
    Saisai Chen
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Saisai Chen
  • Chaohai Wang
    Chaohai Wang
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Chaohai Wang
  • Rui Luo
    Rui Luo
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Rui Luo
  • Junwen Qi
    Junwen Qi
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Junwen Qi
  • Xiuyun Sun
    Xiuyun Sun
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Xiuyun Sun
  • Lianjun Wang
    Lianjun Wang
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    More by Lianjun Wang
  • , and 
  • Jiansheng Li*
    Jiansheng Li
    Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, People’s Republic of China
    *Phone: +86-25-84315351; email: [email protected]
    More by Jiansheng Li
Cite this: Environ. Sci. Technol. 2020, 54, 16, 10289–10300
Publication Date (Web):July 2, 2020
https://doi.org/10.1021/acs.est.0c00914
Copyright © 2020 American Chemical Society
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Abstract

Selective removal of organic pollutants from surface water with high efficiency is crucial in water purification. Here, yolk–shell Co/C nanoreactors (YSCCNs) are facilely synthesized via pyrolysis of controllably etched ZIF-67 by tannic acid, and their degradation performance on multiple pollutants is demonstrated. To present the structure–performance relationship between the designed nanocatalyst and the selective removal of organic pollutants, bisphenol A (BPA) was selected as the targeted pollutant with coexistence of humus acid (HA). For comparison, solid and hollow ZIF-67 derived Co/C nanoparticles denoted as SCCNs and HCCNs, were also tested. The results show that YSCCNs exhibit enhanced BPA degradation rate of 0.32 min–1, which is 23.1% and 45.4% higher than that of HCCNs and SCCNs in HA (10 ppm) system. The essential improvement can be ascribed to the synergetic effects from shell layer (size-exclusion) and core/shell (confinement effect). The degradation mechanism and pathway are further confirmed by radical quenching experiments and liquid chromatography–mass spectrograph (LC–MS), respectively. In addition, some influential factors, including reaction temperature, pH value, and peroxymonosulfate (PMS) dosage are investigated in detail. This work provides a possible way to selectively remove target contaminant from multiple pollutants in complex water system.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c00914.

  • Section S1, characterization; Section S2, preparation of catalysts; Figure S1, XRD of catalyst precursors; Figure S2, SEM images of catalysts and their precursors; Figure S3, the degradation efficiency of 4-CP and TTCH using YSCCNs; Figure S4, The particle size distribution of HA; Figure S5, the degradation rate of SCCNs and YSCCNs for 4-CP and phenol, respectively; Figure S6, the removal efficiency of different catalysts and the effects of initial pH, temperature, and PMS dosage on BPA degradation; Figure S7, the fluorescence emission spectra in different systems; Figure S8, ESI mass spectra of BPA during degradation; Figure S9, the TOC removal of YSCCNs/PMS/BPA and PMS/BPA; Figure S10, cycling stability and leaching of Co ions experiments; Figure S11, the SEM image and XRD pattern of YSCCNs before and after the cycle; Figure S12, before and after used XPS full spectrum of YSCCNs and the high-resolution Co2p XPS spectra of YSCCNs; Figure S13, the degradation efficiency of YSCCNs with different water quality; Table S1, ccomparison of different catalyst for PMS activation; Table S2, the comparison of cycle performance of different catalysts (PDF)

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