General Transformation Law of Chlorinated Acetanilide Herbicides by Reactive Oxidative Species (ROSs) during Photocatalytic Process
General Transformation Law of Chlorinated Acetanilide Herbicides by Reactive Oxidative Species (ROSs) during Photocatalytic Process
复制标题
光催化过程中活性氧化物（ROS）对氯化乙酰苯胺除草剂的一般转化规律
DOI：
10.1016/j.jwpe.2014.11.009
复制
发表时间：
2015-12
影响因子：
7
通讯作者：
Yi, Bing
中科院分区：
文献类型：
--
作者：
Hu, Zhibin;Liu, Huajie;Pang, Huailin;Yi, Bing
选择五种结构相似的氯化乙酰苯胺类除草剂，即甲草胺（Al）、乙草胺（Ac）、丁草胺（Bu）、丙草胺（Pr）和异丙甲草胺（Me），探索光催化过程中活性氧化物种（ROS）转化机制的一般规律。降解动力学顺序为Al>Ac>Me>Bu>Pr，自由基dotOH是引起氯化乙酰苯胺类除草剂降解的主要活性物种。通过计算所提出的降解中间体的前沿电子密度（FED）、点电荷（PC）和Ea，表明与氨基相连的碳原子及其在苯环上的对位很容易与自由基dotOH发生自由基反应，而氯化乙酰苯胺和醚侧链很可能吸附在催化剂表面，然后在初始阶段与光空穴反应。结合HPLC和HPLC/MS/MS的计算结果和鉴定的降解中间体，ROS对这五种氯化乙酰苯胺除草剂提出了三种降解途径，如氯化乙酰苯胺除草剂母体分子上羟基自由基的加成、氮原子上醚侧链的左移和氯化乙酰苯胺的裂解。
Five chlorinated acetanilide herbicides with similar structure, namely alachlor (Al), acetochlor (Ac), butachlor (Bu), propachlor (Pr) and metolachlor (Me), were selected to explore general laws of the transformation mechanism by reactive oxidative species (ROSs) during photocatalytic process. The degradation kinetics followed the order ofAl>Ac>Me>Bu>Pr, and radical dotOH was the main active species for causing the degradation of chlorinated acetanilide herbicides. After calculation of frontier electron densities (FEDs), point charges (PCs) andEaof the proposed degradation intermediates, carbon atom connected to amino group and itspara-position on benzene ring were elucidated to take radical reactions with radical dotOH easily, while the chlorinated acetanilide and ether side chain were likely to be adsorbed on the catalyst surface and then reacted with photohole at the initial stage. Combination of calculated results and identified degradation intermediates by HPLC and HPLC/MS/MS, three degradation pathways were thereby proposed by ROSs for these five chlorinated acetanilide herbicides, such as the addition of hydroxyl radicals to parent molecules of chlorinated acetanilide herbicides, the left of ether side chain on nitrogen atom and the cleavage of chlorinated acetanilide.
登录
查看更多内容
影响因子：
3.3
作者：
Hai Yang;Jiyong Deng;Huajie Liu;Weiwei Yan;Liping Yang;B. Yi
通讯作者：
Hai Yang;Jiyong Deng;Huajie Liu;Weiwei Yan;Liping Yang;B. Yi
影响因子：
6.1
作者：
Dimou, AD;Sakkas, VA;Albanis, TA
通讯作者：
Albanis, TA
影响因子：
5.8
作者：
Tasmin, Rumana;Shimasaki, Yohei;Oshima, Yuji
通讯作者：
Oshima, Yuji
影响因子：
0.7
作者：
N. J. Diepens;S. Pfennig;P. J. Van den Brink;J. Gunnarsson;C. Ruepert;L. Castillo
通讯作者：
N. J. Diepens;S. Pfennig;P. J. Van den Brink;J. Gunnarsson;C. Ruepert;L. Castillo
DOI：
10.1002/jms.3121
发表时间：
2012-12
期刊：
Journal of mass spectrometry : JMS
影响因子：
--
作者：
S. Coffinet;A. Rifai;C. Genty;Yasmine Souissi;S. Bourcier;M. Sablier;S. Bouchonnet
通讯作者：
S. Coffinet;A. Rifai;C. Genty;Yasmine Souissi;S. Bourcier;M. Sablier;S. Bouchonnet