4.7 Article

Enhanced peroxymonosulfate activation via heteroatomic doping defects of pyridinic and pyrrolic N in 2D N-doped carbon nanosheets for BPA degradation

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JOURNAL OF HAZARDOUS MATERIALS
卷 461, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.jhazmat.2023.132626

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Bisphenol A; Carbon nanosheet; Peroxymonosulfate; Pyridinic N; Pyrrolic N

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Understanding the role of intrinsic defects and nonmetallic heteroatom doping defects in activating peroxymonosulfate (PMS) and degrading endocrine-disrupting compounds is crucial for designing efficient carbon catalysts. In this study, N-rich carbon nanosheets (NCs) were synthesized through pyrolysis of a glutamic acid and melamine mixture and were found to enhance PMS activation and bisphenol A (BPA) degradation. The pyridinic and pyrrolic N content in NCs positively correlated with the reaction rate constant (k), indicating their role in generating reactive oxygen species and oxidizing BPA. The NC-activated PMS system with the highest N content demonstrated high efficiency with minimal concentrations of PMS and NC. Excess halide anions increased the reaction rate while minimizing the formation of disinfection byproducts.
Understanding the role of intrinsic defects and nonmetallic heteroatom doping defects in activating peroxymonosulfate (PMS) and subsequently degrading endocrine-disrupting compounds is crucial for designing more efficient carbon catalysts. Therefore, we synthesized N-rich carbon nanosheets (NCs) through pyrolysis of a glutamic acid and melamine mixture and utilized them to activate PMS for bisphenol A (BPA) degradation. Different weight ratios of the above mixtures were allowed for manipulating NCs' defect level and N configuration. The reaction rate constant (k) was significantly positively correlated with the pyridinic and pyrrolic N content, and negatively and weakly positively correlated with graphite N and intrinsic defects, respectively. These findings suggest pyridinic and pyrrolic N, rather than graphitic N and intrinsic defects, enhance PMS activation to generate reactive oxygen species (specifically O center dot-2 and 1O2) and oxidize BPA. The NC-activated PMS system with the highest N content (17.9 atom%) demonstrated a remarkably high k (0.127 min-1) using minimal concentrations of PMS (0.4 mM) and NC (0.15 g/L), highlighting the system's efficiency. Excess halide anions led to significantly increased k with only a limited formation of trichloromethane (disinfection byproducts) in presence of 100 mM Cl-. This study offers novel perspectives on identifying catalytic sites within N-doped carbonaceous materials.

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