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    陈硕

    • 教授     博士生导师   硕士生导师
    • 性别:女
    • 毕业院校:大连理工大学
    • 学位:博士
    • 所在单位:环境学院
    • 学科:环境工程. 环境科学
    • 办公地点:大连理工大学环境学院B717
    • 联系方式:0411-84706263
    • 电子邮箱:shuochen@dlut.edu.cn

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    Fluorine-doped carbon nanotubes as an efficient metal-free catalyst for destruction of organic pollutants in catalytic ozonation

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    论文类型:期刊论文

    第一作者:Wang, Jing

    通讯作者:Quan, X (reprint author), Dalian Univ Technol, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ, Dalian 116024, Peoples R China.

    合写作者:Chen, Shuo,Quan, Xie,Yu, Hongtao

    发表时间:2018-01-01

    发表刊物:CHEMOSPHERE

    收录刊物:SCIE、EI、PubMed

    卷号:190

    页面范围:135-143

    ISSN号:0045-6535

    关键字:Metal-free; Fluorine-doped carbon nanotubes; Catalytic ozonation; Superoxide radicals; Singlet oxygen

    摘要:Metal-free carbon materials have been presented to be potential alternatives to metal-based catalysts for heterogeneous catalytic ozonation, yet the catalytic performance still needs to be enhanced. Doping carbon with non-metallic heteroatoms (e.g., N, B, and F) could alter the electronic structure and electrochemical properties of original carbon materials, has been considered to be an effective method for improving the catalytic activity of carbon materials. Herein, fluorine-doped carbon nanotubes (F-CNTs) were synthesized via a facile method and characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The as-synthesized F-CNTs exhibited notably enhanced catalytic activity towards catalytic ozonation for the degradation of organic pollutants. The oxalic acid removal efficiency of optimized F-CNTs was approximately two times as much as that of pristine CNTs, and even exceeded those of four conventional metal-based catalysts (ZnO, Al2O3, Fe2O3, and MnO2). The XPS and Raman studies confirmed that the covalent C-F bonds were formed at the sp(3) C sites instead of sp(2) C sites on CNTs, not only resulting in high positive charge density of C atoms adjacent to F atoms, but remaining the delocalized pi-system with intact carbon structure of F-CNTs, which then favored the conversion of ozone molecules (O-3) into reactive oxygen species (ROS) and contributed to the high oxalic acid removal efficiency. Furthermore, electron spin resonance (ESR) studies revealed that superoxide radicals (O-2 center dot(-)) and singlet oxygen (O-1(2)) might be the dominant ROS that responsible for the degradation of oxalic acid in these catalytic systems. (C) 2017 Elsevier Ltd. All rights reserved.