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Determination of Instinct Components of Biomass on the Generation of Persistent Free Radicals (PFRs) as Critical Redox Sites in Pyrogenic Chars for Persulfate Activation

  • Wei Wu
    Wei Wu
    State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, P. R. China
    More by Wei Wu
  • Shishu Zhu*
    Shishu Zhu
    School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, P. R. China
    *Email: [email protected]
    More by Shishu Zhu
  • Xiaochen Huang
    Xiaochen Huang
    School of Agriculture, Sun Yat-Sen University, Guangzhou 510275, P. R. China
  • Wei Wei
    Wei Wei
    Centre for Technology in Water and Wastewater, School of Civil and Environmental Engineering, University of Technology Sydney, Sydney, NSW 2007, Australia
    More by Wei Wei
  • Chao Jin
    Chao Jin
    School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, P. R. China
    More by Chao Jin
  • , and 
  • Bing-Jie Ni*
    Bing-Jie Ni
    Centre for Technology in Water and Wastewater, School of Civil and Environmental Engineering, University of Technology Sydney, Sydney, NSW 2007, Australia
    *Email: [email protected]
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Cite this: Environ. Sci. Technol. 2021, 55, 11, 7690–7701
Publication Date (Web):May 17, 2021
https://doi.org/10.1021/acs.est.1c01882
Copyright © 2021 American Chemical Society
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Abstract

Persulfate (PS) activation on biochar (BC) is a promising technology for degrading the aqueous organic contaminants. However, the complexity of activation mechanisms and components in biomass that used to produce BC makes it difficult to predict the performance of PS activation. In this study, we employed eight sludges as the representative biomass that contained absolutely different organic or inorganic components. Results showed that the elemental composition, surface properties, and structures of the sludge-derived BCs (SBCs) clearly depended on the inherent components in the sludges. The intensities of persistent free radicals (PFRs) in the electron paramagnetic resonance (EPR) correlated positively with N-containing content of sludges as electron shuttle, but negatively with the metal content as electron acceptor. Linking with PFRs as crucial sites of triggering a radical reaction, a poly-parameter relationship of predicting PS activation for organic degradation using the sludge components was established (kobs,PN = 0.004 × Cprotein + 0.16 × CM–0.895 −0.118). However, for the PS activation on those SBCs without PFRs, this redox process only relied on the sorption or conductivity-related characteristics, not correlating with the content of intrinsic components in biomass but with pyrolysis temperatures. This study provided insightful information of predicting the remediation efficiency of PS activation on BCs and further understanding the fate of contaminants and stoichiometric efficiency of oxidants in a field application.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.1c01882.

  • Total protein and polysaccharide examination (Text S1); total COD examination (Text S2); digestion of sludge (Text S3); determination of charge-transfer resistance and electron-donating capacity (Text S4); EPR spectroscopy experiments (Text S5); discussions about the variances of H/C and O/C (Text S6); discussions about results of FTIR (Text S7); discussions about the sources of sludge (Text S8); Tables S1–S4; and Figures S1–S20 (PDF)

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