Enhanced peroxymonosulfate activation by Cu-doped LaFeO3 with rich oxygen vacancies: Compound-specific mechanisms

[Display omitted] •Cu doping significantly increased the catalytic activity of LFO toward PMS.•The enhanced activity of LFCO is attributable to abundant oxygen vacancies.•The degradation reaction mechanism of pharmaceuticals is compound specific.•Intermediates were identified and SDZ decay pathways...

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Veröffentlicht in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2022-05, Vol.435, p.134882, Article 134882
Hauptverfasser: Rao, Yongfang, Zhang, Yuanyuan, Fan, Jiahui, Wei, Gaoling, Wang, Dan, Han, Fuman, Huang, Yu, Croué, Jean-Philippe
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Sprache:eng
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Zusammenfassung:[Display omitted] •Cu doping significantly increased the catalytic activity of LFO toward PMS.•The enhanced activity of LFCO is attributable to abundant oxygen vacancies.•The degradation reaction mechanism of pharmaceuticals is compound specific.•Intermediates were identified and SDZ decay pathways are proposed.•Toxicity decrease was observed during SDZ degradation. The degradation reaction mechanisms of organic pollutants by peroxymonosulfate (PMS) activation processes remain controversial. In this study, Cu-doped LaFeO3 samples were prepared and used as heterogeneous catalysts of PMS for the degradation of pharmaceuticals. Compared to LaFeO3 (LFO), the increased catalytic activity of LaFe1-xCuxO3 (LFCO) samples was observed, among which LFCO-7.5 exhibited the best performance. The enhanced catalytic activity of LFCO-7.5 was attributable to the generation of abundant oxygen vacancies. Hydroxyl radicals, sulfate radicals, superoxide and singlet oxygen were detected in the LFCO-7.5/PMS system. However, selective effects of radical scavengers on the degradation of different pharmaceuticals and selective reactivity of singlet oxygen toward different pharmaceuticals indicate the existence of compound-specific degradation mechanisms in the LFCO-7.5/PMS system. Furthermore, possible degradation pathways of SDZ and the toxicity evolution were investigated during sulfadiazine (SDZ) degradation. This study further enhances our knowledge on the degradation reaction mechanisms of organic pollutants in PMS activation processes.
ISSN:1385-8947
1873-3212
DOI:10.1016/j.cej.2022.134882