零价铁活化分子氧矿化三嗪类除草剂策略
详细信息    查看官网全文
摘要
阿特拉津(Atrizine,2-氯-4-乙胺基-6-异丙胺基-1,3,5-三嗪)作为抑制农田杂草生长的一种三嗪类的除草剂,三嗪环的开环及矿化是三嗪类除草剂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[1]。本研究旨在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,避免脱氯上羟基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。利用LC-MS/MS以及GC-MS监测到Fe@Fe2O3/Ni(II)/air体系中脱氯上氢是阿特拉津降解的重要过程。此外,利用拉曼光谱分析阿特拉津降解不同时间的中间产物,当反应时间为34 h时,位于682、962、990、1250、1547、1598 cm-1处三嗪环上振动峰[2]全部消失,几乎只存在体系外加的SO4-的振动峰,说明原本阿特拉津中三嗪环的状态已经被破坏,阿特拉津极有可能在镍离子存在的铁活化分子氧体系中三嗪环开环降解。
The destruction and mineralization of the atrazine 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 degradation of s-triazine herbicides at mild conditions and the final oxidation product is cyanuric acid with s-triazine ring.This study aims to develop a novel molecular oxygen activation system for the breaking and minerazation of s-triazine herbicide with the utilization of nanometer zero-valent iron.In the 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 generating stable cyanuric acid through reaction between hydroxoy radicals and s-triazine herbicide,leading to breaking and mineralization of s-triazine herbicide via non-cyanuric acid pathway,thus total destruction of s-triazine herbicide at room temperature and pressure over zero-valent iron could be obtained.
引文
[1]Pelizzetti,E.;Maurino,V.;Minero,C.;Carlin,V.;Tosato,M.L.;Pramauro,E.;Zerbinati,O.,Photocatalytic degradation of atrazine and other s-triazine herbicides.Environ.Sci.Tech.1990,24,(10),1559-1565.
    [2]Costa,J.C.S.;Ando,R.A.;Camargo,P.H.C.;Corio,P.,Understanding the Effect of Adsorption Geometry over Substrate Selectivity in the Surface-Enhanced Raman Scattering Spectra of Simazine and Atrazine.J.Phys.Chem.C.2011,115,(10),4184-4190.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700