Catalytic Removal of Aqueous Contaminants on N-Doped Graphitic Biochars: Inherent Roles of Adsorption and Nonradical Mechanisms

  • Shishu Zhu
    Shishu Zhu
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, 73 Huanghe Road, Harbin 150090, PR China
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    More by Shishu Zhu
  • Xiaochen Huang
    Xiaochen Huang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, 73 Huanghe Road, Harbin 150090, PR China
  • Fang Ma
    Fang Ma
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, 73 Huanghe Road, Harbin 150090, PR China
    More by Fang Ma
  • Li Wang*
    Li Wang
    State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, 73 Huanghe Road, Harbin 150090, PR China
    *Phone: +86-188-46180363. E-mail: [email protected]
    More by Li Wang
  • Xiaoguang Duan*
    Xiaoguang Duan
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    *Phone: +61-892-665403. E-mail: [email protected]
  • , and 
  • Shaobin Wang
    Shaobin Wang
    Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth, Western Australia 6845, Australia
    More by Shaobin Wang
Cite this: Environ. Sci. Technol. 2018, 52, 15, 8649–8658
Publication Date (Web):July 20, 2018
https://doi.org/10.1021/acs.est.8b01817
Copyright © 2018 American Chemical Society
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Abstract

Environmentally friendly and low-cost catalysts are important for the rapid mineralization of organic contaminants in powerful advanced oxidation processes (AOPs). In this study, we reported N-doped graphitic biochars (N-BCs) as low-cost and efficient catalysts for peroxydisulfate (PDS) activation and the degradation of diverse organic pollutants in water treatment, including Orange G, phenol, sulfamethoxazole, and bisphenol A. The biochars at high annealing temperatures (>700 °C) presented highly graphitic nanosheets, large specific surface areas (SSAs), and rich doped nitrogen. In particular, N-BC derived at 900 °C (N-BC900) exhibited the highest degradation rate, which was 39-fold and 6.5-fold of that on N-BC400 and pristine biochar, respectively, and the N-BC900 surpassed most popular metal or nanocarbon catalysts. Different from the radical-based oxidation in N-BC400/PDS via the persistent free radicals (PFRs), singlet oxygen and nonradical pathways (surface-confined activated persulfate–carbon complexes) were discovered to dominate the oxidation processes in N-BC900/PDS. Moreover, the adsorption of organics was determined to be the key step determining reaction rate, revealing that the pre-adsorption of reactants significantly accelerated the nonradical oxidation pathway. This study not only provides robust and cheap carbonaceous materials for environmental remediation but also enables the first insight into the graphitic biochar-based nonradical catalysis.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b01817.

  • Additional details on materials and methods, the results, and their discussion. Tables showing surface porosity and state percentages. Figures showing SEM images, XPS spectra, XRD patterns, Raman spectra, PDS activation, OG removal efficiencies, FTIR spectra, the effect of catalyst and PDS concentration, the scavenge effect of ethanol, EPR spectra, catalytic stability, HPLC–MS results, adsorption kinetics, kinetic and Langmuir isotherm models, and oxidative degradation rate. (PDF)

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