三嗪环的开环及矿化是三嗪类除草剂农药在环境中彻底消除的必要步骤.温和条件下高级氧化技术氧化三嗪类除草剂的最终产物是三聚氰酸,无法实现其开环矿化.本课题组拟通过在纳米零价铁活化分子氧氧化体系引入镍离子,促进氢自由基产生,调控体系中活性物种种类,诱导三嗪类除草剂加氢脱氯,避免羟基自由基加羟基脱氯生成极其稳定的三聚氰酸中间产物,优化三嗪类除草剂的降解途径,实现常温常压下纳米零价铁活化分子氧矿化三嗪类除草剂.本文计划系统考察体系中界面电子转移途径、分子氧活化机理、溶剂水的作用、活性物种的种类,深入分析活性物种生成和消亡途径;研究除草剂污染物的降解特性以及各种活性物种在三嗪类除草剂C—Cl和C—N键断裂过程中的作用,揭示不同活性物种与典型三嗪类除草剂的相互作用规律,阐明三嗪类除草剂降解和三嗪环开环等机理,为发展绿色高效农药污染控制技术提供理论支持.
The destruction and mineralization of the s-triazine ring is the final and key step for the complete removal of environmental s-triazine herbicide pollutants. Advanced oxidation technologies can not break down the s-triazine ring when the degradation of s-triazine herbicides is carried at mild conditions and the final oxidation product is cyanuric acid with s-triazine ring. This project aims to develop a novel molecular oxygen activation system for the breaking and minerazation of s-triazine herbicides with the utilization of nanometer zero-valent iron. In this novel system,nickel ions with catalytic activity of hydrogen will be introduced in order to adjust the types and quantities of active species and avoid the generation of stable cyanuric acid through the reactions between hydroxoy radicals and s-triazine herbicide,leading to the breaking and mineralization of s-triazine herbicide via a non-cyanuric acid pathway,thus the total destruction of s-triazine herbicide at room temperature and pressure over zero-valent iron could be achieved. The pathway of interfacial electron transfer,the active species generatation,and the types and formation of active species will be investigated systematically. The characteristics of herbicide pollutants degradation and the breaking mechanism of C—N and C—Cl bonds of s-triazine by different active species will be studied in detail. This project could provide theoretical support for the development of green and efficient pollution control technology.