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LaMnO 中铜促进过一硫酸盐活化以调控磺胺甲恶唑降解中的活性氧物种。

Copper in LaMnO to promote peroxymonosulfate activation by regulating the reactive oxygen species in sulfamethoxazole degradation.

机构信息

School of Environmental Studies, China University of Geosciences, Wuhan 430074, PR China.

Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, PR China.

出版信息

J Hazard Mater. 2021 Jun 5;411:125163. doi: 10.1016/j.jhazmat.2021.125163. Epub 2021 Jan 16.

Abstract

Perovskites with flexible texture structures and excellent catalytic properties have attracted considerable attention in peroxymonosulfate (PMS) activation for addressing organic contaminants in water. In this study, the role of copper to promote PMS activation performance of LaMnO was investigated. 100% sulfamethoxazole (SMX) degradation and 34% mineralization were achieved over copper doped LaMnO while only 60% SMX was removed without TOC removal by LaMnO. Especially, compared with LaMnO, the pseudo-first-order reaction rate constant was increased by 8.30 times when the atomic ratio of Cu/Mn was 1:3. It proved that only O was generated in LaMnO while O, especially •OH and SO• were all detected in Cu-LaMnO/PMS system. The characterization results showed that Cu induced the formation of LaMnO and LaCuO heterostructure with enhanced content of relatively low-valence Mn and Cu and abundant oxygen vacancies (OVs). Hence, the efficient PMS activation by Cu-LaMnO was due to regulating the produced reactive oxygen species (ROS). A radical dominant instead of O involved PMS activation mechanism over LaMnO-LaCuO was proposed for efficient degradation of SMX. Finally, the possible degradation pathways of SMX were discussed based on HPLC-MS analysis. This study provided a new insight of improving the catalytic activity of perovskites in PMS activation in water treatment.

摘要

具有柔性结构和优异催化性能的钙钛矿在过一硫酸盐 (PMS) 活化中引起了相当大的关注,可用于处理水中的有机污染物。在本研究中,考察了铜在促进 LaMnO 活化过一硫酸盐性能方面的作用。铜掺杂 LaMnO 可实现 100%的磺胺甲恶唑 (SMX) 降解和 34%的矿化,而 LaMnO 则无法去除 TOC,仅去除了 60%的 SMX。特别是,与 LaMnO 相比,当 Cu/Mn 原子比为 1:3 时,其假一级反应速率常数提高了 8.30 倍。这证明在 LaMnO 中仅生成了 O,而在 Cu-LaMnO/PMS 体系中检测到了 O、特别是 •OH 和 SO•。表征结果表明,Cu 诱导了 LaMnO 和 LaCuO 异质结构的形成,增加了相对低价态 Mn 和 Cu 的含量以及丰富的氧空位 (OVs)。因此,Cu-LaMnO 对 PMS 的高效活化归因于调节产生的活性氧物质 (ROS)。提出了一种以自由基为主导而不是 O 参与的过一硫酸盐活化机制,用于高效降解 SMX。最后,根据 HPLC-MS 分析讨论了 SMX 的可能降解途径。本研究为提高水相处理中过一硫酸盐活化的钙钛矿的催化活性提供了新的见解。

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