包覆型络合态Fe(II)控释强化UV/过硫酸盐技术降解水中离子载体抗生素的效能与机理

Ionophore Antibiotics, as a class of pharmaceutical pollutants, has been attracted worldwide attention recently. This project aims to prepare a sustained release microcapsules-like encapsulated ferrous complex (EFC) with environment-friendly polymer and soluble Fe(II) complex by molten suspension and cooling method. The releasing rate of Fe(II) can be controlled by adjusting the preparation parameters. Efficient degradation of IPAs by EFC enhanced-UV/persulfate process (EFC-UV/PS) is expected to realize through gradient Fe(II) release and improved regeneration of Fe(II). The interaction of Fe(II) complex with persulfate and Fe(II) regeneration mechanism are explored via ATR-FTIR, confocal Raman spectroscop, and competitive kinetics method. Further investigation on key influence factors, the detoxification efficiency, degradation pathway and kinetic model is conducted. The implementation of this project is expected to provide a new environmentally method for degradation and detoxification of IPAs，as well as a novel way for practical application of sulfate radical based-AOTs.

离子载体抗生素(IPAs)是一类新近受到关注的污染物。本课题利用熔化悬浮冷凝技术，制成以环境友好聚合物为包覆壁材以水溶性Fe(II)络合物为芯材的Fe(II)控释材料(EFC)，通过控制包覆制备条件调节Fe(II)的释放速率，利用EFC梯度释放络合态Fe(II)强化过硫酸盐(PS)分解，协同紫外强化Fe(II)再生，实现IPAs在EFC-UV/PS体系中的高效降解。采用傅里叶变换衰减全反射红外光谱、共聚焦拉曼光谱、电子顺磁共振技术和Ferrozine法，结合竞争动力学手段，探明络合态Fe(II)与PS的作用机理及其再生历程。深入研究EFC-UV/PS技术降解IPAs的关键影响因素、生物毒性去除规律、降解机理及降解数学模型。本项目为水中IPAs的有效降解和毒性消除提供环境友好的新方法，也为硫酸根自由基高级氧化技术的推广应用提供了一条新途径。

离子载体抗生素(Ionophore antibiotics, IPAs)对生态环境和公共安全带来了极大的风险。为了解决目前大多数技术对IPAs降解及解毒效率偏低的问题，本项目利用硫酸根自由基极强的氧化性，提出了包覆型络合态Fe(II)原位控释技术与UV/PMS技术耦合这样一种光助硫酸根自由基高级氧化技术。以地表水中检出频率较高的IPAs为研究对象，制备了包覆型络合态Fe(II)控释材料，探求其控释性能协同UV/PS技术达到最佳降解效能的匹配关系，解析了包覆型络合态Fe(II)控释强化UV/PS技术降解IPAs的基本规律，明确了关键影响因素(水质参数和工艺参数，揭示了体系中主要活性物种的生成与转化规律，分析降解产物，阐明降解路径及脱毒机理。最后，构建并优化了IPAs的降解动力学模型。本项目的成功实施为水中IPAs类有机污染物的去除和控制提供技术支持和理论指导，而且有助于发展以硫酸根自由基为基础的新型高级氧化技术，从而推动其在污染控制与环境修复中的应用。