Carbonization of camphor sulfonic acid and melamine to N,S-co-doped carbon for sulfamethoxazole degradation via persulfate activation: Nonradical dominant pathway

•·NSC-750 outperformed the nitrogen-free SC-750 in persulfate activation.•·96% removal, 69% mineralization, and 98% PS utilization rate were achieved.•·Hybridized EPR spectra, coupling 1O2 and unpaired electron signal, was found.•·Pyridinic N, thiophene-S, and structural defects were the active site...

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Veröffentlicht in:Separation and purification technology 2021-12, Vol.279, p.119723, Article 119723
Hauptverfasser: Sun, Wei, Pang, Kangfeng, Ye, Feng, Pu, Mengjie, Zhou, Chengzhi, Huang, Haiming, Zhang, Qichun, Niu, Junfeng
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Sprache:eng
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Zusammenfassung:•·NSC-750 outperformed the nitrogen-free SC-750 in persulfate activation.•·96% removal, 69% mineralization, and 98% PS utilization rate were achieved.•·Hybridized EPR spectra, coupling 1O2 and unpaired electron signal, was found.•·Pyridinic N, thiophene-S, and structural defects were the active sites.•·Nonradical 1O2 dominated the oxidization of SMX. A nonradical dominant degradation process via N,S-co-doped carbon-catalyzed persulfate (PS) activation was reported. The camphor sulfonic acid acted as both carbon and sulfur source, and melamine served as nitrogen source. The introduction of N atom into S-doped carbon created new defective sites and N active species. Accordingly, the resulting NSC-750 showed an enhanced catalytic activity (0.0348 min−1), with 5.8-folds higher SMX removal efficiency than that of SC-650 (0.006 min−1). 96% removal, 69% mineralization, and 98% PS decomposition rate were achieved. The NSC-750/PS system could work effectively over a wide pH range of 3–9. While carbonate (CO32–) played an opposite role in degrading SMX. Both radical and nonradical pathway were involved in SMX degradation. Therein, 1O2 played a critical role while .OH, SO4.-, and electron transfer exerted a minor contribution. It was assumed that pyridine N and thiophene S are responsible for the production of SO4.-; structural defect and C = O contributed to the formation of 1O2 and electron-transfer process, respectively; partial 1O2 was originated from the conversation of O2.-. In addition, NSC-750/PS system was capable of degrading other contaminants (bisphenol A, ciprofloxacin, and rhodamine B et al). The obtained hybrid EPR spectra, coupling with 1O2 and unpaired electron signal of catalyst, broadens our horizon to better distinguish the reactive species. This work facilitates the application of N,S-co-doped carbon in nonradical-dominated antibiotics remediation, and deepens the understanding of catalytic mechanism and active sites.
ISSN:1383-5866
1873-3794
DOI:10.1016/j.seppur.2021.119723