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中空多壳 CoO 作为纳米反应器来激活过一硫酸盐以实现高效降解卡马西平:一种减少纳米催化剂团聚的新策略。

Hollow multi-shelled CoO as nanoreactors to activate peroxymonosulfate for highly effective degradation of Carbamazepine: A novel strategy to reduce nano-catalyst agglomeration.

机构信息

Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang 310058, China; Zhejiang Provincial Key Laboratory of Organic Pollution Process and Control, Hangzhou, Zhejiang 310058, China.

出版信息

J Hazard Mater. 2022 Apr 5;427:127890. doi: 10.1016/j.jhazmat.2021.127890. Epub 2021 Nov 24.

Abstract

Reducing the agglomeration of nano-catalysts to retain the active catalytic sites is crucial for the advanced oxidation processes (AOPs) of peroxymonosulfate activation in wastewater treatments. Herein, CoO hollow multi-shelled structures (HoMSs) were successfully prepared as the nanoreactors to reduce the agglomeration of nano-catalysts in catalytic reaction. Compared with single-shelled and double-shelled CoO HoMSs, triple-shelled CoO HoMSs (TS-CoO) exhibited best catalytic performance and the carbamazepine (5 mg L) degradation reached 100% within 30 min. The hollow multi-shelled structures showed a significant role in reducing the agglomeration of catalysts. The value of hydrodynamic diameter/true particle size of TS-CoO was 1.58, which meant TS-CoO could be regarded as a single dispersion or two together in aqueous solution. The shells of TS-CoO supported each other and outer shells could protect the inner ones, hence the stability increased. Besides, the hollow cavity between shells reduced the mass diffusion resistance and increased the contact of reactants with active sites. Mechanism studies showed sulfate radicals (SO) played a leading role in the degradation of carbamazepine. This work provided an effective way to reduce the agglomeration and retain the active sites of cobalt-based catalysts in AOPs, so as to balance the conflict between the reactivity and stability of nano-catalysts.

摘要

在废水处理中,通过过一硫酸盐(PMS)活化的高级氧化工艺(AOPs)来保留活性催化位点,减少纳米催化剂的团聚是至关重要的。本文中,成功制备了 CoO 中空多壳结构(HoMSs)作为纳米反应器,以减少催化反应中纳米催化剂的团聚。与单壳和双壳 CoO HoMSs 相比,三壳 CoO HoMSs(TS-CoO)表现出最佳的催化性能,在 30 分钟内,卡马西平(5mg/L)的降解率达到 100%。中空多壳结构在减少催化剂团聚方面发挥了重要作用。TS-CoO 的水动力直径/真实粒径值为 1.58,这意味着在水溶液中,TS-CoO 可以被视为单个分散体或两个聚集在一起。TS-CoO 的壳层相互支撑,外壳可以保护内部壳层,因此稳定性增加。此外,壳层之间的中空腔减少了质量扩散阻力并增加了反应物与活性位点的接触。机理研究表明,硫酸根自由基(SO)在卡马西平的降解中起主导作用。这项工作为减少 AOPs 中钴基催化剂的团聚和保留活性位点提供了一种有效方法,从而平衡纳米催化剂的反应性和稳定性之间的冲突。

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