Yang Xue, Yu Hai, Hong Liang, Huang Zhihang, Zeng Qinda, Yao Xiao, Qiu Yinyuan
School of Ecological Environment and Urban Construction, Fujian University of Technology, Fuzhou 350118, China.
School of Mechanical and Automotive Engineering, Fujian University of Technology, Fuzhou 350118, China.
Molecules. 2025 Jun 21;30(13):2690. doi: 10.3390/molecules30132690.
In recent years, extensive attention has been paid to advanced oxidation processes (AOPs) with peracetic acid (PAA), a widely used disinfectant, using transition metal ions for the degradation of organic contaminants within water environments. Mn(II) has been widely used as an effective homogeneous transition metal catalyst for oxidant activation, but it has shown poor performances with PAA. Since the stability of manganese species can be enhanced through the addition of ligands, this study systematically investigated a novel AOP for the oxidation of carbamazepine (CBZ) using an Mn(II)/PAA system with several different ligands added. The reactive species were explored through UV-vis spectrometry, scavengers, and probe compounds. The results suggest that Mn(III)-ligand complexes and other high-valent Mn species (Mn(V)) were generated and contributed obviously toward efficient CBZ oxidation, while radicals like CHCO and CHCO were minor contributors. The oxidation efficiency of Mn(II)/PAA/ligands depended highly on ligand species, as ethylene diamine tetraacetic acid (EDTA) and oxalate (SO) could promote the oxidation of CBZ, while pyrophosphate (PPP) showed modest enhancement. The results obtained here might contribute to the removal of residue pharmaceuticals under manganese-rich waters and also shed light on PAA-based AOPs that could help broaden our present knowledge of manganese chemistry for decontamination in water treatment.
近年来，使用过渡金属离子通过过氧乙酸（PAA，一种广泛使用的消毒剂）在水环境中降解有机污染物的高级氧化过程（AOPs）受到了广泛关注。锰（II）已被广泛用作氧化剂活化的有效均相过渡金属催化剂，但它与PAA的性能不佳。由于通过添加配体可以提高锰物种的稳定性，本研究系统地研究了一种新型的AOP，即使用添加了几种不同配体的Mn（II）/PAA体系氧化卡马西平（CBZ）。通过紫外可见光谱、清除剂和探针化合物探索了活性物种。结果表明，生成了Mn（III）-配体络合物和其他高价锰物种（Mn（V）），它们对CBZ的高效氧化有明显贡献，而CHCO和CHCO等自由基的贡献较小。Mn（II）/PAA/配体的氧化效率高度依赖于配体种类，因为乙二胺四乙酸（EDTA）和草酸盐（SO）可以促进CBZ的氧化，而焦磷酸盐（PPP）的促进作用适中。这里获得的结果可能有助于去除富锰水中的残留药物，也为基于PAA的AOPs提供了线索，这有助于拓宽我们目前关于锰化学在水处理中去污的知识。
