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pH Dependence of Arsenic Oxidation by Rice-Husk-Derived Biochar: Roles of Redox-Active Moieties

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    pH Dependence of Arsenic Oxidation by Rice-Husk-Derived Biochar: Roles of Redox-Active Moieties
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    • Delai Zhong
      Delai Zhong
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong P.R. China
      More by Delai Zhong
      Orcidhttp://orcid.org/0000-0003-1394-8346
    • Yi Jiang
      Yi Jiang
      Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong P.R. China
      More by Yi Jiang
      Orcidhttp://orcid.org/0000-0002-4193-0330
    • Zezhou Zhao
      Zezhou Zhao
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      More by Zezhou Zhao
    • Linling Wang*
      Linling Wang
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      *Phone: +86 27 87792159; fax: +86 27 87792101; e-mail: [email protected]
      More by Linling Wang
      Orcidhttp://orcid.org/0000-0001-7468-9064
    • Jing Chen
      Jing Chen
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      More by Jing Chen
      Orcidhttp://orcid.org/0000-0002-7243-0806
    • Shupeng Ren
      Shupeng Ren
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      More by Shupeng Ren
    • Zhenhua Liu
      Zhenhua Liu
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      More by Zhenhua Liu
    • Yanrong Zhang*
      Yanrong Zhang
      School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, P.R. China
      *E-mail: [email protected]
      More by Yanrong Zhang
      Orcidhttp://orcid.org/0000-0002-8793-090X
    • Daniel C. W. Tsang
      Daniel C. W. Tsang
      Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong P.R. China
      More by Daniel C. W. Tsang
      Orcidhttp://orcid.org/0000-0002-6850-733X
    • John C. Crittenden
      John C. Crittenden
      Brook Byers Institute of Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
      More by John C. Crittenden
      Orcidhttp://orcid.org/0000-0002-9048-7208
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2019, 53, 15, 9034–9044
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    https://doi.org/10.1021/acs.est.9b00756
    Published July 2, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    Biochars have demonstrated great potential for water decontamination and soil remediation; however, their redox reactivity toward trace contaminants and the corresponding redox-active moieties (RAMs, i.e., phenolic −OH, semiquinone-type persistent free radicals (PFRs), and quinoid C═O) remain poorly understood. Here we investigated the roles of the RAMs on biochar in oxidation of As(III) under varying pH and O2 conditions. The results showed that the promoted oxidation of As(III) by the RAMs is strongly pH dependent. Under acidic and neutral conditions, only the oxidation of As(III) by •OH and H2O2 produced from activation of O2 by phenolic −OH and semiquinone-type PFRs occurred. In contrast, the oxidation by semiquinone-type PFRs, quinoid C═O, and H2O2 (if O2 was introduced) appeared under alkaline conditions. This pH-dependent oxidation behavior was attributed to the varying redox activities of RAMs, as confirmed by multiple characterization and validation experiments using biochar with tuned RAMs compositions, as well as thermodynamics evaluation. Our findings provide new insights into the roles of the RAMs on biochar in the promoted oxidation of trace As(III) over a broader pH range under both anoxic and oxic conditions. This study also paves a promising way to oxidize As(III) with biochar.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.9b00756.

    • Materials and chemicals; preparation of rBC400 and oBC400; data collection and analysis of FTIR, EPR, XPS, and modified Boehm titration; As adsorption analysis; comparison of As(III) oxidation in different systems; proposed Eh-pH diagrams for the biochar/As(III)/O2 systems (PDF)

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    Cite this: Environ. Sci. Technol. 2019, 53, 15, 9034–9044
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