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MoTiCT@Co高效活化过一硫酸盐以持续去除新兴微污染物:类芬顿反应中钼空位介导的活化作用

Efficient activation of peroxymonosulfate by MoTiCT@Co for sustained emerging micropollutant removal: Mo vacancy-mediated activation in Fenton-like reactions.

作者信息

Zhang Siling, Liu Dezhu, Lin Zili, Chen Ping, Wang Yishun, Liu Linsheng, Xu Zihong, Jian Junle, Lv Wenying, Liu Guoguang

机构信息

Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China.

Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China.

出版信息

J Colloid Interface Sci. 2025 Apr 15;684(Pt 1):60-74. doi: 10.1016/j.jcis.2024.12.233. Epub 2024 Dec 31.

DOI:10.1016/j.jcis.2024.12.233
PMID:39787808
Abstract

Developing advanced heterogeneous catalysts through structural modifications effectively enhances the catalytic activity of non-homogeneous catalysts for removing emerging micropollutants (EMPs). In this study, MoTiCT@Co with Mo vacancies was synthesized using the Lewis molten salt method, which efficiently activates peroxymonosulfate (PMS) and continuously degrades EMPs in water. The abundant Mo vacancy structure in the material acts as an anchoring site for Co nanoparticles and a co-catalytic site for Fenton-like reactions, enabling PMS adsorption and activation. Furthermore, Mo facilitates the redox cycling of Co/Co through electron transfer. Mo vacancy-mediated activation in Fenton-like reactions enabled the MoTiCT@Co/PMS system to achieve superior degradation efficiency for sulfamethoxazole (SMX) and several other EMPs, with the SMX degradation rate being 52.7 times higher than that of the MoTiAlC/PMS system. The system exhibited robust resistance to various anionic species and maintained high activity over a wide pH range. The MoTiCT@Co /PMS system degrades EMPs in water through both free radical (SO and •OH) and non-radical (O) mechanisms, enhancing EMPs removal from complex water environments. This study aims to develop an efficient and sustainable heterogeneous catalyst, offering a viable solution for the long-term and effective degradation of EMPs in water.

摘要

通过结构修饰开发先进的非均相催化剂可有效提高非均相催化剂去除新兴微污染物(EMPs)的催化活性。在本研究中,采用路易斯熔盐法合成了具有Mo空位的MoTiCT@Co,其能有效活化过一硫酸盐(PMS)并持续降解水中的EMPs。材料中丰富的Mo空位结构作为Co纳米颗粒的锚定位点和类芬顿反应的共催化位点,实现PMS的吸附和活化。此外,Mo通过电子转移促进Co/Co的氧化还原循环。类芬顿反应中Mo空位介导的活化使MoTiCT@Co/PMS体系对磺胺甲恶唑(SMX)和其他几种EMPs具有卓越的降解效率,SMX降解率比MoTiAlC/PMS体系高52.7倍。该体系对各种阴离子具有强大的抗性,在较宽的pH范围内保持高活性。MoTiCT@Co /PMS体系通过自由基(SO和•OH)和非自由基(O)机制降解水中的EMPs,提高了复杂水环境中EMPs的去除率。本研究旨在开发一种高效且可持续的非均相催化剂,为水中EMPs的长期有效降解提供可行方案。

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