{"title":"LaCo0.95Mo0.05O3/CeO2 复合材料可通过 Co3+/Co2+ 循环促进过氧单硫酸盐的有效活化,实现硫酸羟氯喹的高效降解。","authors":"Huiwen Ding, Tianqi Jiang, Haijiao Xie, Jianqiao Wang, Pengfei Xiao","doi":"10.1016/j.jcis.2024.09.174","DOIUrl":null,"url":null,"abstract":"<p><p>Hydroxychloroquine sulfate (HCQ) is extensively utilized due to its numerous therapeutic effects. Because of its properties of high solubility, persistence, bioaccumulation, and biotoxicity, HCQ can potentially affect water bodies and human health. In this study, the LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub> material was successfully prepared by the sol-gel process, and it was applied to the experiment of degrading HCQ by activating peroxymonosulfate (PMS). The results of characterization analysis showed that LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub> material had good stability, and the problem of particle agglomeration had been solved to some extent. Compared with LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub> material, it had a larger specific surface area and more oxygen vacancies, which was helpful to improve the catalytic activity for PMS. Under optimal conditions, the LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub>/PMS system degraded 95.5 % of HCQ in 10 min. The singlet oxygen, superoxide radicals, and sulfate radicals were the main radicals for HCQ degradation. The addition of Mo<sup>6+</sup>/Mo<sup>4+</sup> and Ce<sup>4+</sup>/Ce<sup>3+</sup> promoted the redox cycle of Co<sup>3+</sup>/Co<sup>2+</sup> and enhanced the degradation rate of HCQ. Based on density functional theory and experimental analysis, three HCQ degradation pathways were proposed. The analysis of T.E.S.T software showed that the toxicity of HCQ was obviously reduced after degradation. The LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub>/PMS system displayed excellent reusability and the ability to remove pollutants in a wide range of real-world aqueous environments, with the ability to treat a wide range of pharmaceutical wastewater. In summary, this study provides some ideas for developing heterogeneous catalysts for advanced oxidation systems and provide an efficient, simple, and low-cost method for treating pharmaceutical wastewater that has good practical application potential.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"678 Pt C","pages":"1151-1169"},"PeriodicalIF":9.4000,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>/CeO<sub>2</sub> composite can promote the effective activation of peroxymonosulfate via Co<sup>3+</sup>/Co<sup>2+</sup> cycle and realize the efficient degradation of hydroxychloroquine sulfate.\",\"authors\":\"Huiwen Ding, Tianqi Jiang, Haijiao Xie, Jianqiao Wang, Pengfei Xiao\",\"doi\":\"10.1016/j.jcis.2024.09.174\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Hydroxychloroquine sulfate (HCQ) is extensively utilized due to its numerous therapeutic effects. Because of its properties of high solubility, persistence, bioaccumulation, and biotoxicity, HCQ can potentially affect water bodies and human health. In this study, the LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub> material was successfully prepared by the sol-gel process, and it was applied to the experiment of degrading HCQ by activating peroxymonosulfate (PMS). The results of characterization analysis showed that LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub> material had good stability, and the problem of particle agglomeration had been solved to some extent. Compared with LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub> material, it had a larger specific surface area and more oxygen vacancies, which was helpful to improve the catalytic activity for PMS. Under optimal conditions, the LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub>/PMS system degraded 95.5 % of HCQ in 10 min. The singlet oxygen, superoxide radicals, and sulfate radicals were the main radicals for HCQ degradation. The addition of Mo<sup>6+</sup>/Mo<sup>4+</sup> and Ce<sup>4+</sup>/Ce<sup>3+</sup> promoted the redox cycle of Co<sup>3+</sup>/Co<sup>2+</sup> and enhanced the degradation rate of HCQ. Based on density functional theory and experimental analysis, three HCQ degradation pathways were proposed. The analysis of T.E.S.T software showed that the toxicity of HCQ was obviously reduced after degradation. The LaCo<sub>0.95</sub>Mo<sub>0.05</sub>O<sub>3</sub>-CeO<sub>2</sub>/PMS system displayed excellent reusability and the ability to remove pollutants in a wide range of real-world aqueous environments, with the ability to treat a wide range of pharmaceutical wastewater. In summary, this study provides some ideas for developing heterogeneous catalysts for advanced oxidation systems and provide an efficient, simple, and low-cost method for treating pharmaceutical wastewater that has good practical application potential.</p>\",\"PeriodicalId\":351,\"journal\":{\"name\":\"Journal of Colloid and Interface Science\",\"volume\":\"678 Pt C\",\"pages\":\"1151-1169\"},\"PeriodicalIF\":9.4000,\"publicationDate\":\"2025-01-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Colloid and Interface Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jcis.2024.09.174\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/9/19 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Colloid and Interface Science","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.jcis.2024.09.174","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/9/19 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
LaCo0.95Mo0.05O3/CeO2 composite can promote the effective activation of peroxymonosulfate via Co3+/Co2+ cycle and realize the efficient degradation of hydroxychloroquine sulfate.
Hydroxychloroquine sulfate (HCQ) is extensively utilized due to its numerous therapeutic effects. Because of its properties of high solubility, persistence, bioaccumulation, and biotoxicity, HCQ can potentially affect water bodies and human health. In this study, the LaCo0.95Mo0.05O3-CeO2 material was successfully prepared by the sol-gel process, and it was applied to the experiment of degrading HCQ by activating peroxymonosulfate (PMS). The results of characterization analysis showed that LaCo0.95Mo0.05O3-CeO2 material had good stability, and the problem of particle agglomeration had been solved to some extent. Compared with LaCo0.95Mo0.05O3 material, it had a larger specific surface area and more oxygen vacancies, which was helpful to improve the catalytic activity for PMS. Under optimal conditions, the LaCo0.95Mo0.05O3-CeO2/PMS system degraded 95.5 % of HCQ in 10 min. The singlet oxygen, superoxide radicals, and sulfate radicals were the main radicals for HCQ degradation. The addition of Mo6+/Mo4+ and Ce4+/Ce3+ promoted the redox cycle of Co3+/Co2+ and enhanced the degradation rate of HCQ. Based on density functional theory and experimental analysis, three HCQ degradation pathways were proposed. The analysis of T.E.S.T software showed that the toxicity of HCQ was obviously reduced after degradation. The LaCo0.95Mo0.05O3-CeO2/PMS system displayed excellent reusability and the ability to remove pollutants in a wide range of real-world aqueous environments, with the ability to treat a wide range of pharmaceutical wastewater. In summary, this study provides some ideas for developing heterogeneous catalysts for advanced oxidation systems and provide an efficient, simple, and low-cost method for treating pharmaceutical wastewater that has good practical application potential.
期刊介绍:
The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality.
Emphasis:
The journal emphasizes fundamental scientific innovation within the following categories:
A.Colloidal Materials and Nanomaterials
B.Soft Colloidal and Self-Assembly Systems
C.Adsorption, Catalysis, and Electrochemistry
D.Interfacial Processes, Capillarity, and Wetting
E.Biomaterials and Nanomedicine
F.Energy Conversion and Storage, and Environmental Technologies