Research Group of Water Pollution Control and Water Reclamation, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, PR China.
Research Group of Water Pollution Control and Water Reclamation, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, PR China.
Chemosphere. 2023 Oct;339:139672. doi: 10.1016/j.chemosphere.2023.139672. Epub 2023 Jul 28.
Sulfate radical-based advanced oxidation processes (SR-AOPs) is considered as one of the most promising technologies for antibiotic pollution. In this study, a core-shell catalyst of cobalt-manganese oxide derived from CoMn-MOFs coating by MgAl-LDH (Co/Mn@LDH) was synthesized for peroxymonosulfate (PMS) activation to degrade sulfamethoxazole (SMX). Degradation efficiency of nearly 100% and a mineralization efficiency of 68.3% for SMX were achieved in Co/Mn@LDH/PMS system. Mn species and out shell MgAl-LDH greatly suppressed the cobalt ions leaching, which only 23 μg/L Co ions were detected by ICP after the reaction. SO was identified as dominant reactive species in the system. Furthermore, the possible reactive sites of SMX were predicted by the density functional theory (DFT) calculations. And the intermediates of SMX were detected by LC-MS and the degradation pathway was proposed based on the results above. The ECOSAR results suggested the intermediates of SMX showed a relatively low toxicity compared to SMX, indicating huge potential of utilization of Co/Mn@LDH in SR-AOPs system.
基于硫酸根自由基的高级氧化工艺（SR-AOPs）被认为是抗生素污染最有前途的技术之一。在这项研究中，合成了一种由 CoMn-MOFs 涂层衍生的钴锰氧化物核壳催化剂 Co/Mn@LDH，用于过一硫酸盐（PMS）的活化以降解磺胺甲恶唑（SMX）。在 Co/Mn@LDH/PMS 体系中，SMX 的降解效率接近 100%，矿化效率达到 68.3%。Mn 物种和外壳 MgAl-LDH 极大地抑制了钴离子的浸出，反应后仅检测到 23μg/L 的 Co 离子。SO 被确定为该体系中的主要活性物质。此外，通过密度泛函理论（DFT）计算预测了 SMX 的可能反应位点。通过 LC-MS 检测到 SMX 的中间产物，并根据上述结果提出了降解途径。ECOSAR 结果表明，与 SMX 相比，SMX 的中间产物显示出相对较低的毒性，这表明 Co/Mn@LDH 在 SR-AOPs 系统中的利用具有巨大的潜力。
