Electronic Structure Modulation of Graphitic Carbon Nitride by Oxygen Doping for Enhanced Catalytic Degradation of Organic Pollutants through Peroxymonosulfate Activation

  • Yaowen Gao
    Yaowen Gao
    Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China
    More by Yaowen Gao
  • Yue Zhu
    Yue Zhu
    Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China
    More by Yue Zhu
  • Lai Lyu
    Lai Lyu
    Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China
    More by Lai Lyu
  • Qingyi Zeng
    Qingyi Zeng
    Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China
    More by Qingyi Zeng
  • Xueci Xing
    Xueci Xing
    Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China
    More by Xueci Xing
  • , and 
  • Chun Hu*
    Chun Hu
    Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China
    *Phone: +86-20-39346609; fax: +86-10-62923541; e-mail: [email protected]/[email protected]
    More by Chun Hu
Cite this: Environ. Sci. Technol. 2018, 52, 24, 14371–14380
Publication Date (Web):November 14, 2018
https://doi.org/10.1021/acs.est.8b05246
Copyright © 2018 American Chemical Society
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Abstract

Oxygen-doped graphitic carbon nitride (O–CN) was fabricated via a facile thermal polymerization method using urea and oxalic acid dihydrate as the graphitic carbon nitride precursor and oxygen source, respectively. Experimental and theoretical results revealed that oxygen doping preferentially occurred on the two-coordinated nitrogen positions, which create the formation of low and high electron density areas resulting in the electronic structure modulation of O–CN. As a result, the resultant O–CN exhibits enhanced catalytic activity and excellent long-term stability for peroxymonosulfate (PMS) activation toward the degradation of organic pollutants. The O–CN with modulated electronic structure enables PMS oxidation over the electron-deficient C atoms for the generation of singlet oxygen (1O2) and PMS reduction around the electron-rich O dopants for the formation of hydroxyl radical (OH) and sulfate radical (SO4•–), in which 1O2 is the major reactive oxygen species, contributing to the selective reactivity of the O–CN/PMS system. Our findings not only propose a novel PMS activation mechanism in terms of simultaneous PMS oxidation and reduction for the production of nonradical and radical species but also provide a valuable insight for the development of efficient metal-free catalysts through nonmetal doping toward the persulfate-based environmental cleanup.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b05246.

  • Tables showing element contents, BET surface areas and pore volumes as well as XPS spectra results; figures showing molecular structures of various organic pollutants, XPS survey spectra, TOC removal, effect of common inorganic anions, XRD patterns of fresh and used O–CN, activation of persulfate by O–CN, FTIR spectra of O–CN after different reactions, and effect of scavengers and degradation of BPA in N2-saturated atmosphere (PDF)

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