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一种新型的三维石墨烯基钴锰双金属层状双氢氧化物:在水溶液中光助过一硫酸盐活化降解磺胺甲恶唑的形成机理及性能

A novel 3-dimensional graphene-based cobalt-manganese bimetallic layered double hydroxide:Formation mechanism and performance in photo-assisted permonosulfate-activated degradation of sulfamethoxazole in aqueous solution.

作者信息

Liu Zhibo, Duan Xiaoyue, Sarmah Ajit K, Zhao Xuesong, Ren Xin, Sun Bo

机构信息

College of Environmental Science and Engineering, Jilin Normal University, Haifeng Street, Tiexi Dist, Siping, 136000, China.

Key Laboratory of Environmental Materials and Pollution Control, Education Department of Jilin Province, Siping, 136000, China.

出版信息

Environ Pollut. 2023 Nov 1;336:122397. doi: 10.1016/j.envpol.2023.122397. Epub 2023 Aug 17.

Abstract

Sulfamethoxazole (SMX) is a common antibiotic used mainly for bacterial treatment. In this study, a novel three-dimensional cobalt-manganese bimetallic layered double hydroxide graphene hydrogel (CoMn-LDHs/rGO) has been prepared for photo-assisted permonosulfate (PMS)-activated degradation of SMX in water. Compared with the CoMn-LDHs/rGO + PMS and CoMn-LDHs/rGO + Vis systems, the degradation effect of CoMn-LDHs/rGO + PMS + Vis system is the best, and the degradation effect of CoMn-LDHs/rGO system could reach more than 98% under the optimal conditions. After 10 cycles, the catalytic degradation performance of CoMn-LDHs/rGO system remained good, while effectively preventing the leaching of metal ions. Based on the synergistic effect of photocatalysis and PMS oxidation, electron spin resonance spectroscopy and quenching experiments showed that three active substances (•OH, •SO and O) were involved in the degradation of SMX. Density functional theory and liquid chromatography-mass spectrometry (LC-MS) results further proposed the SMX degradation transformation calculation. As expected, the study of the reaction mechanism of 3D CoMn-LDHs/rGO assisted PMS activation under visible light provides an efficient and rapid method for the sustainable degradation of pollutants in water system.

摘要

磺胺甲恶唑(SMX)是一种主要用于细菌治疗的常见抗生素。在本研究中,制备了一种新型的三维钴 - 锰双金属层状双氢氧化物石墨烯水凝胶(CoMn-LDHs/rGO),用于光辅助过一硫酸盐(PMS)活化降解水中的SMX。与CoMn-LDHs/rGO + PMS和CoMn-LDHs/rGO + Vis体系相比,CoMn-LDHs/rGO + PMS + Vis体系的降解效果最佳,在最佳条件下CoMn-LDHs/rGO体系的降解效果可达98%以上。经过10次循环后,CoMn-LDHs/rGO体系的催化降解性能保持良好,同时有效防止了金属离子的浸出。基于光催化和PMS氧化的协同作用,电子自旋共振光谱和猝灭实验表明三种活性物质(•OH、•SO和O)参与了SMX的降解。密度泛函理论和液相色谱 - 质谱(LC-MS)结果进一步提出了SMX降解转化计算。正如预期的那样,对可见光下三维CoMn-LDHs/rGO辅助PMS活化反应机理的研究为水体系中污染物的可持续降解提供了一种高效快速的方法。

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