Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, 650500, Kunming, Yunnan, China.
College of Chemistry, Dalian University of Technology, 116024, Dalian, Liaoning, China.
J Hazard Mater. 2018 Jul 5;353:26-34. doi: 10.1016/j.jhazmat.2018.02.034. Epub 2018 Feb 20.
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 HO and dissolved oxygen resulting in the formation of OH that was primarily responsible for the degradation of sulfamethoxazole. The reactions of 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 Fc-catalyzed 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.
对于激活氧化剂以产生用于深度修复被抗生素污染的水体的反应性物种，易得且高效的催化剂是必不可少的。在这项研究中，引入二茂铁（Fc）来建立用于磺胺类抗生素降解的非均相光芬顿系统，以磺胺甲恶唑作为代表性抗生素。结果表明，Fc 催化的光芬顿系统对磺胺甲恶唑的去除效果显著。电子自旋共振和自由基清除实验验证了 Fc 向 HO 和溶解氧的光诱导电子转移过程，从而形成了 OH，这是磺胺甲恶唑降解的主要原因。OH 与磺胺甲恶唑的亚结构模型化合物的反应表明，苯胺部分是磺胺甲恶唑的优先反应位点，这通过在 Fc 催化的光芬顿系统中形成羟化产物和磺胺甲恶唑的二聚体得到了验证。即使在复杂的水基质中，这种非均相光芬顿系统也显示出有效的降解效率，并且 Fc 通过多次使用催化剂表现出长期稳定性。这些结果表明，Fc 催化的光芬顿氧化可能是修复含抗生素废水的有效方法。
