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Defluorination and Mineralization of Difluorophenols in Water by Anodic Contact Glow Discharge Electrolysis

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Abstract

Anodic contact glow discharge electrolysis (CGDE) is a DC-excited atmospheric pressure discharge, in which a steady non-thermal plasma is generated locally between the surface of an electrolytic solution and an anode in contact with it. The I–U characteristics of CGDE were investigated. The plasma temperatures were estimated to be in the range, 1373–2045 K. Hydroxyl radicals and hydrogen peroxide were the main oxidants generated by CGDE. The hydrogen peroxide concentration reached 31.2 mmol/L (mM) in a phosphate buffer solution without organic substrates. During CGDE, the DFPs and the corresponding total organic carbon (TOC) in water were consumed. Most of the fluorine atoms in the DFPs were converted to fluoride ions, and the fluoride concentration increased steadily. An analysis of the hydroxylation of DFPs suggested that the hydroxyl radicals generated by CGDE were the key species responsible for the degradation of DFPs, and the possible mechanistic routes of the mineralization of DFPs are proposed. The disappearance of DFPs and the TOC as well as the defluorination of the DFPs followed first-order kinetics. The rate of TOC disappearance was relatively constant: 1.00 ± 0.05 × 10−2 min−1. The order of disappearance of the DFPs was 2,6-DFP > 2,3-DFP > 2,5-DFP > 2,4-DFP > 3,4-DFP > 3,5-DFP. In contrast, the order of defluorination of the DFPs was 2,5-DFP > 2,3-DFP > 2,6-DFP > 2,4-DFP > 3,4-DFP > 3,5-DFP. Overall, the order of the reaction rates for each DFP was kDFP > kdF > kTOC.

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Acknowledgments

This work was supported by the National Natural Science Foundation of China (Grant No. 51308276), Scientific Research Foundation for Doctors of Liaoning Province (Grant No. 20141123), Growth Plan for Distinguished Young Scholars in Colleges and Universities of Liaoning Province China (LJQ2015055), Anshan Science and Technology Program Project (Grant No. 2961), the National Natural Science Foundation of China (51102126), Innovative Research Team in Colleges and Universities of Liaoning Province China (LT2014007), Natural Science Foundation of Liaoning Province, China (2015020634).

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Authors and Affiliations

  1. School of Chemical Engineering, University of Science and Technology Liaoning, Anshan, 114051, China

    Haiming Yang, Xiaotong Zhao, Baigang An, Lixiang Li & Shaoyan Wang

  2. Graduate School of Engineering, Saitama Institute of Technology, 1690 Fusaiji, Fukaya, Saitama, 369-0293, Japan

    Giya Mengen & Meguru Tezuka

  3. National Marine Environmental Monitoring Center, Dalian, 116023, China

    Maowei Ju

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  1. Haiming Yang
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  2. Xiaotong Zhao
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  3. Giya Mengen
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Correspondence to Haiming Yang or Maowei Ju.

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Yang, H., Zhao, X., Mengen, G. et al. Defluorination and Mineralization of Difluorophenols in Water by Anodic Contact Glow Discharge Electrolysis. Plasma Chem Plasma Process 36, 993–1009 (2016). https://doi.org/10.1007/s11090-016-9715-4

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  • DOI: https://doi.org/10.1007/s11090-016-9715-4

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