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ZnO-CoO对双氯芬酸的催化降解:主要中间体的鉴定及降解途径

Catalytic degradation of diclofenac by ZnO-CoO: identification of major intermediates and degradation pathway.

作者信息

Fergani Soumia, Zazoua Hanane, Saadi Adel, Badri Fatma Zohra, Boudjemaa Amel, Bachari Khaldoun

机构信息

Laboratory of Natural Gas Chemistry, Faculty of Chemistry, USTHB, El Alia, Algiers, Po Box 32, Algeria.

Centre de Recherche Scientifique Et Technique en Analyses Physico-Chimiques, CP 42004, Bou-Ismail, Tipaza, Algeria.

出版信息

Environ Sci Pollut Res Int. 2025 Jan;32(4):1971-1984. doi: 10.1007/s11356-024-35713-5. Epub 2025 Jan 3.

Abstract

ZnO-CoO material was successfully synthesized by the co-precipitation method and used as a catalyst for the removal of diclofenac sodium (DCF). ZnO-CoO exhibited higher catalytic activity in the catalytic process compared to the photocatalytic processes. Under optimum conditions, the activation of peroxymonosulfate (PMS) by ZnO-CoO achieved approximately 99% removal of DCF, confirming the effective adsorption and activation of PMS. Quenching experiments indicated that the reactive oxygen species (ROS) responsible for the degradation of DCF by the ZnO-CoO/PMS system are singlet oxygen (O) and superoxide radicals (O). The activation of PMS by ZnO-CoO was associated with the coexistence and interaction between Co(II) and Co(III), as well as the formation of oxygen vacancies (V) in ZnO. Cobalt leaching was negligible, and the degradation rate remained constant after four cycles, indicating the excellent stability and reusability of the ZnO-Co₃O₄ catalyst. Additionally, eight degradation products of DCF were identified by LC-ESI-MS, and their toxicity was evaluated using ECOSAR software (version 2.2). In conclusion, the ZnO-CoO/PMS system is a promising catalytic process for the degradation of organic molecules.

摘要

通过共沉淀法成功合成了ZnO-CoO材料,并将其用作去除双氯芬酸钠(DCF)的催化剂。与光催化过程相比,ZnO-CoO在催化过程中表现出更高的催化活性。在最佳条件下,ZnO-CoO对过一硫酸盐(PMS)的活化实现了约99%的DCF去除率,证实了对PMS的有效吸附和活化。猝灭实验表明,ZnO-CoO/PMS体系中负责DCF降解的活性氧物种(ROS)是单线态氧(O)和超氧自由基(O)。ZnO-CoO对PMS的活化与Co(II)和Co(III)之间的共存和相互作用以及ZnO中氧空位(V)的形成有关。钴浸出可忽略不计,四个循环后降解率保持恒定,表明ZnO-Co₃O₄催化剂具有优异的稳定性和可重复使用性。此外,通过LC-ESI-MS鉴定了DCF的八种降解产物,并使用ECOSAR软件(版本2.2)评估了它们的毒性。总之,ZnO-CoO/PMS体系是一种有前途的有机分子降解催化过程。

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