Mohaned Hammad, Steven Angel, Ahmed K. Al-kamal, Anam Asghar, Mena-Alexander Kräenbring, Adil Amin, Haakon T.A. Wiedemann, Amin S. Amin, Vineetha Vinayakumar, Torsten C. Schmidt, Christopher W.M. Kay, Doris Segets, Hartmut Wiggers
{"title":"Spray-flame synthesis of LaCo0.2Mn0.8O3 for selective peroxymonosulfate activation into singlet oxygen towards efficient degradation of carbamazepine","authors":"Mohaned Hammad, Steven Angel, Ahmed K. Al-kamal, Anam Asghar, Mena-Alexander Kräenbring, Adil Amin, Haakon T.A. Wiedemann, Amin S. Amin, Vineetha Vinayakumar, Torsten C. Schmidt, Christopher W.M. Kay, Doris Segets, Hartmut Wiggers","doi":"10.1016/j.psep.2024.12.060","DOIUrl":null,"url":null,"abstract":"Improving the efficiency and stability of heterogeneous catalysts is essential for effectively utilizing peroxymonosulfate activation in industrial wastewater treatment. Perovskite ABO<ce:inf loc=\"post\">3</ce:inf> catalysts with high structural flexibility have gained considerable attention in the peroxymonosulfate activation for the removal of hazardous organic compounds from wastewater. However, there is still considerable potential for catalytic enhancement due to the ease of tailoring its composition and structure. Herein, we introduce a scalable method to synthesize LaCo<ce:inf loc=\"post\">0.2</ce:inf>Mn<ce:inf loc=\"post\">0.8</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> with the aim of improving the catalytic performance. Interestingly, LaCo<ce:inf loc=\"post\">0.2</ce:inf>Mn<ce:inf loc=\"post\">0.8</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> with abundant oxygen vacancies and improved dispersion stability exhibited enhanced catalytic degradation of carbamazepine compared to the LaMnO<ce:inf loc=\"post\">3</ce:inf> and LaCoO<ce:inf loc=\"post\">3</ce:inf> catalysts in the peroxymonosulfate activation system. The partial substitution of manganese by cobalt in LaMnO<ce:inf loc=\"post\">3</ce:inf> leading to the LaCo<ce:inf loc=\"post\">0.2</ce:inf>Mn<ce:inf loc=\"post\">0.8</ce:inf>O<ce:inf loc=\"post\">3</ce:inf>+peroxymonosulfate system maintains a relatively high performance over repeated usage. Furthermore, the LaCo<ce:inf loc=\"post\">0.2</ce:inf>Mn<ce:inf loc=\"post\">0.8</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> catalyst exhibited excellent catalytic performance and stability across a broad pH range (3–9). Electron paramagnetic resonance and radical quenching experiment tests demonstrated singlet oxygen (<ce:sup loc=\"post\">1</ce:sup>O<ce:inf loc=\"post\">2</ce:inf>) as the primary active species for carbamazepine degradation in the LaCo<ce:inf loc=\"post\">0.2</ce:inf>Mn<ce:inf loc=\"post\">0.8</ce:inf>O<ce:inf loc=\"post\">3</ce:inf>+ peroxymonosulfate system, while free radicals, such as sulfate radicals (SO<ce:inf loc=\"post\">4</ce:inf><ce:sup loc=\"post\">•–</ce:sup>), hydroxyl radicals (<ce:sup loc=\"post\">•</ce:sup>OH), and superoxide radicals (O<ce:inf loc=\"post\">2</ce:inf><ce:sup loc=\"post\">•–</ce:sup>), played a minor role in the carbamazepine removal. Taken together, this research provides significant insight into the effect of B-site substitution on the catalytic performance of perovskite catalysts.","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"202 1","pages":""},"PeriodicalIF":6.9000,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Process Safety and Environmental Protection","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.psep.2024.12.060","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Improving the efficiency and stability of heterogeneous catalysts is essential for effectively utilizing peroxymonosulfate activation in industrial wastewater treatment. Perovskite ABO3 catalysts with high structural flexibility have gained considerable attention in the peroxymonosulfate activation for the removal of hazardous organic compounds from wastewater. However, there is still considerable potential for catalytic enhancement due to the ease of tailoring its composition and structure. Herein, we introduce a scalable method to synthesize LaCo0.2Mn0.8O3 with the aim of improving the catalytic performance. Interestingly, LaCo0.2Mn0.8O3 with abundant oxygen vacancies and improved dispersion stability exhibited enhanced catalytic degradation of carbamazepine compared to the LaMnO3 and LaCoO3 catalysts in the peroxymonosulfate activation system. The partial substitution of manganese by cobalt in LaMnO3 leading to the LaCo0.2Mn0.8O3+peroxymonosulfate system maintains a relatively high performance over repeated usage. Furthermore, the LaCo0.2Mn0.8O3 catalyst exhibited excellent catalytic performance and stability across a broad pH range (3–9). Electron paramagnetic resonance and radical quenching experiment tests demonstrated singlet oxygen (1O2) as the primary active species for carbamazepine degradation in the LaCo0.2Mn0.8O3+ peroxymonosulfate system, while free radicals, such as sulfate radicals (SO4•–), hydroxyl radicals (•OH), and superoxide radicals (O2•–), played a minor role in the carbamazepine removal. Taken together, this research provides significant insight into the effect of B-site substitution on the catalytic performance of perovskite catalysts.
期刊介绍:
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