4.7 Article

Enhanced peroxymonosulfate decomposition into ?OH and 1O2 for sulfamethoxazole degradation over Se doped g-C3N4 due to induced exfoliation and N vacancies formation

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ELSEVIER
DOI: 10.1016/j.seppur.2021.118664

关键词

Metal-free catalyst; Graphitic carbon nitride; PMS activation; Selenium; Non radical and radical reaction; SMX degradation

资金

  1. National Natural Science Foundation of China [51878633, 41773126, 41807200]
  2. Foundation for Innovative Research Groups of the National Natural Science Foundation of China [41521001]
  3. Fundamental Research Funds for the Central Universities
  4. China Postdoctoral Science Foundation [2020M672443]

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The introduction of selenium into graphitic carbon nitride (g-C3N4) can enhance its performance in activating peroxymonosulfate (PMS), leading to more efficient degradation of organic pollution caused by antibiotics. The Se-doped g-C3N4 (Se-g-C3N4) showed a significant increase in degradation rate compared to bulk g-C3N4, attributed to the enhanced PMS decomposition and electron transfer process. This work provides a new strategy for improving the PMS activation performance of g-C3N4 by regulating electron distribution and increasing exposure of reactive sites.
The development of low-cost and facile synthesized metal-free peroxymonosulfate (PMS) activation catalysts is paramount important for the practical remediation of organic pollution caused by antibiotics. Graphitic carbon nitride (g-C3N4) as a promising alternative, to improve its PMS activation performance, we proposed an efficient method to prepare exfoliated Se doped g-C3N4 (Se-g-C3N4) with 0.095 wt% Se and more exposed reactive N vacancies through the thermal polycondensation of melamine and Se powder at 550 ?. The results proved that 93.0% of sulfamethoxazole (SMX) can be degraded over Se-g-C3N4 with PMS in 180 min, and the corresponding degradation rate constant of 0.0149 min? 1 was even 4-fold higher than that of bulk g-C3N4 (0.0039 min-1). It was found that more 1O2 was generated and ?OH was further identified because of the enhanced PMS selfdecomposition process, especially PMS reduction via electron transfer from Se-g-C3N4. The introduction of Se atom in g-C3N4 structure not only induced the formation of nitrogen vacancies to modulate the electron distribution of g-C3N4, but also favored the exfoliation of inter-facial stacking to increase the exposure of active sites due to the large atomic radius of Se. Hence, this work offered a new strategy for improving the PMS activation performance of g-C3N4 by regulating its electron deficiency and exposing more reactive N vacancies simultaneously.

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