Enhanced Perfluorooctanoic Acid Degradation by Electrochemical Activation of Sulfate Solution on B/N Codoped Diamond

  • Yanming Liu
    Yanming Liu
    Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, P. R. China
    More by Yanming Liu
  • Xinfei Fan
    Xinfei Fan
    College of Environmental Science and Engineering, Dalian Maritime University, Dalian 116024, P. R. China
    More by Xinfei Fan
  • Xie Quan*
    Xie Quan
    Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, P. R. China
    *E-mail: [email protected]
    More by Xie Quan
  • Yaofang Fan
    Yaofang Fan
    Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, P. R. China
    More by Yaofang Fan
  • Shuo Chen
    Shuo Chen
    Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, P. R. China
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  • , and 
  • Xueyang Zhao
    Xueyang Zhao
    Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education, China), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, P. R. China
    More by Xueyang Zhao
Cite this: Environ. Sci. Technol. 2019, 53, 9, 5195–5201
Publication Date (Web):April 8, 2019
https://doi.org/10.1021/acs.est.8b06130
Copyright © 2019 American Chemical Society
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Abstract

Electrochemical oxidation based on SO4•– and OH generated from sulfate electrolyte is a cost-effective method for degradation of persistent organic pollutants (POPs). However, sulfate activation remains a great challenge due to lack of active and robust electrodes. Herein, a B/N codoped diamond (BND) electrode is designed for electrochemical degradation of POPs via sulfate activation. It is efficient and stable for perfluorooctanoic acid (PFOA) oxidation with first-order kinetic constants of 2.4 h–1 and total organic carbon removal efficiency of 77.4% (3 h) at relatively low current density of 4 mA cm–2. The good activity of BND mainly originates from a B and N codoping effect. The PFOA oxidation rate at sulfate electrolyte is significantly enhanced (2.3–3.4 times) compared with those at nitrate and perchlorate electrolytes. At sulfate, PFOA oxidation rate decreases slightly in the presence of OH quencher while it declines significantly with SO4•– and OH quenchers, indicate both SO4•– and OH contribute to PFOA oxidation but SO4•– contribution is more significant. On the basis of intermediates analysis, a proposed mechanism for PFOA degradation is that PFOA is oxidized to shorter chain perfluorocarboxylic acids gradually by SO4•– and OH until it is mineralized.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b06130.

  • XPS spectrum of BND, PFOA removal kinetics of BND at sulfate, chronopotentiometric curve, SEM images and XRD spectra of BDD and NDD, B/N contents of three electrodes, and PFOA removal kinetics of BDD and NDD at sulfate and BND at nitrate and perchlorate (PDF)

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