Ferrocene-catalyzed heterogeneous Fenton-like degradation mechanisms and pathways of antibiotics under simulated sunlight: A case study of sulfamethoxazole
Ferrocene-catalyzed heterogeneous Fenton-like degradation mechanisms and pathways of antibiotics under simulated sunlight: A case study of sulfamethoxazole
复制标题
模拟阳光下二茂铁催化抗生素异质芬顿降解机制和途径：以磺胺甲恶唑为例
DOI：
10.1016/j.jhazmat.2018.02.034
复制
发表时间：
2018-07-05
影响因子：
13.6
通讯作者：
Tian, Senlin
中科院分区：
文献类型：
--
作者：
Li, Yingjie;Zhang, Biaojun;Tian, Senlin
容易获得和有效的催化剂是活化氧化剂产生活性物种以深度修复被抗生素污染的水体所必需的。以磺胺甲恶唑为代表，引入二茂铁（Fe），建立了非均相光Fenton体系降解磺胺类抗生素。结果表明，在Fe催化光Fenton体系中，磺胺甲恶唑的去除效果较好。电子自旋共振（ESR）和自由基清除实验证实，光诱导Fe ~（2+）向H_2O_2和溶解氧的电子转移过程导致中心点OH的形成，而中心点OH是磺胺甲恶唑降解的主要原因。中心点OH与磺胺甲恶唑亚结构模型化合物的反应揭示了苯胺部分是磺胺甲恶唑的优选反应位点，并通过在Fe（CN）催化的光Fenton体系中磺胺甲恶唑羟基化产物和二聚体的生成证实了这一点。这种多相光Fenton体系即使在复杂的水基质中也表现出有效的降解效率，并且通过使用催化剂多次循环，Fc表现出长期稳定性。这些结果表明，Fc催化的光Fenton氧化可能是一种有效的方法来修复含抗生素废水。
Readily-available and efficient catalyst is essential for activating oxidants to produce reactive species for deeply remediating water bodies contaminated by antibiotics. In this study, Ferrocene (Fc) was introduced to establish a heterogeneous photo-Fenton system for the degradation of sulfonamide antibiotics, taking sulfamethoxazole as a representative. Results showed that the removal of sulfamethoxazole was effective in Fc-catalyzed photo-Fenton system. Electron spin resonance and radical scavenging experiments verified that there was a photoindued electron transfer process from Fc to H2O2 and dissolved oxygen resulting in the formation of center dot OH that was primarily responsible for the degradation of sulfamethoxazole. The reactions of center dot OH with substructure model compounds of sulfamethoxazole unveiled that aniline moiety was the preferable reaction site of sulfamethoxazole, which was verified by the formation of hydroxylated product and the dimer of sulfamethoxazole in Fccatalyzed photo-Fenton system. This heterogeneous photo-Fenton system displayed an effective degradation efficiency even in a complex water matrices, and Fc represented a long-term stability by using the catalyst for multiple cycles. These results demonstrate that Fc-catalyzed photo-Fenton oxidation may be an efficient approach for remediation of wastewater containing antibiotics.