新型硅酸盐复合基膜强化臭氧氧化水中多种单苯环止痛类药物的特性和机制研究

Control technologies of pharmaceuticals and personal care products (PPCPs) in water have become a hot research topic. Among the PPCPs, analgesic pharmaceuticals with single phenyl ring have some problems to control in water, such as low concentration, slow metabolism. Thus, it is of great significance to remove them by chemical oxidation technology. In previous study, a low cost silicate composite based microfiltration membrane was successfully fabricated and it had an obvious advantage of removal trace organic pollutants in water by enhancing ozonation. Therefore, in this research, the pre-studied membrane-enhanced ozonation system is used to degrade a series of aqueous analgesic pharmaceuticals with single phenyl ring structure. Degradation laws are also studied. Firstly, the analgesic pharmaceuticals are separately degraded in ozone-alone and ozone-membrane trials. Based on the result, differences of removal efficiency and some important influence factors can be achieved in the two processes. Secondly, through a comparative study of removal processes and degradation byproducts, a structure-activity relationship between the substituent species and the removal efficiencies can be established, and the mechanism of membrane-enhanced ozonation process can also be discovered. Finally, operation conditions of the membrane-enhanced ozonation process are studied. Depending on the outcome, a complete set of technical parameters is proposed for the process, which provides a technical basis for effectively removal of analgesic pharmaceuticals in actual water.

药品及个人护理品（PPCPs）在水体中的控制技术逐渐成为研究热点。在PPCPs中，单苯环止痛类药物因在水环境中浓度低、生物代谢慢，利用化学氧化技术去除具有研究意义。申请人前期成功制备出一种低成本硅酸盐复合基微滤膜，并发现其具有强化臭氧氧化水中微量有机污染物的显著优势。因此，本项目将前期开发的膜强化臭氧氧化技术应用于水中多种单苯环的止痛类药物的去除研究，探索该类药物降解的规律。本项目对目标物分别进行单独臭氧氧化和膜强化臭氧氧化的比较研究，分析两种工艺中目标物去除率的差异及关键影响因素。比较目标物降解过程及产物，构建目标物苯环上取代基种类和位置与其氧化降解之间的构效关系，探究膜强化臭氧氧化此类药物的机制。考察膜强化臭氧氧化单苯环止痛类药物的工艺运行条件，提出该技术氧化目标物的成套工艺技术参数，为有效控制实际水体中的单苯环止痛类药物提供技术支持。

药品及个人护理品（PPCPs）在水体中的控制技术逐渐成为研究热点。在PPCPs中，单苯环药物因在水环境中浓度低、生物代谢慢，利用化学氧化技术去除具有研究意义。项目负责人前期成功制备出一种低成本硅酸盐复合膜，并发现其具有强化臭氧氧化水中微量有机污染物的显著优势。因此，本项目将前期开发的膜强化臭氧氧化技术应用于水中多种单苯环药物的去除研究，探索该类药物降解的规律。本项目对水杨酸、乙酰水杨酸、布洛芬和多氯硝基苯共四种药物分别进行了单独臭氧氧化和膜强化臭氧氧化的比较研究，分析了两种工艺中目标物去除效果的差异及关键影响因素；比较了目标物降解过程及产物生成历程的区别，构建了目标物苯环上取代基种类和位置与其氧化降解之间的构效关系；探究了膜强化臭氧氧化单苯环药物的机制，发现了体系内以羟基自由基为主的关键氧化因子；以UV-O3和FeOOH-O3两种典型羟基自由基氧化体系为例，比较了膜强化臭氧体系与传统高级氧化体系在单苯环药物降解方面的异同，证明提出的膜-O3体系是一种有竞争力的新型高级氧化体系；最后考察了膜强化臭氧氧化单苯环药物的工艺运行条件，提出了该技术氧化目标物的成套工艺技术参数，为有效控制实际水体中的单苯环药物提供了技术支持。