文献类型：期刊文献

英文题名：Sulfate radical-based oxidation of the aminopyralid and picloram herbicides: The role of amino group on pyridine ring

作者：Yang, Xuerui[1,4];Cao, Xue[1];Zhang, Li[1];Wu, Yanlin[2,3];Zhou, Lei[1];Xiu, Guangli[1];Ferronato, Corinne[4];Chovelon, Jean-Marc[4]

机构：[1]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai Environm Protect Key Lab Environm Stand, Shanghai 200237, Peoples R China;[2]Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China;[3]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[4]Univ Claude Bernard Lyon 1, Univ Lyon, CNRS, UMR 5256,IRCELYON, 2 Ave Albert Einstein, F-69626 Villeurbanne, France

年份：2021

卷号：405

外文期刊名：JOURNAL OF HAZARDOUS MATERIALS

收录：;EI(收录号：20204309403870);WOS:【SCI-EXPANDED(收录号:WOS:000616162500001)】；

基金：This work was supported by the National Natural Science Foundation of China (No. 21806037).

语种：英文

外文关键词：Herbicides; Amino group; Self-coupling products; Azo derivatives; Sulfate radical

摘要：The widespread utilization of pesticides has attracted increasing attention to their environmental impacts and effective removal strategies. In the present study, the degradation of herbicides picloram (PCLO) and amino-pyralid (AMP) with similar structures were investigated systematically by thermo activated persulfate. Overweight SO4 center dot- was determined to be the predominant oxidizing species by quenching experiment. Obtained by laser-flash photolysis (LFP), reaction rate constants of SO4 center dot- towards AMP and PCLO were determined at 1.56 x 10(9) M-1 s(-1) and 1.21 x 10(9) M-1 s(-1), respectively. Product analysis revealed that both substances underwent similar oxidation paths, namely, successive oxidation on pyridine ring and formation of coupling-products as well as further hydroxylation and decarboxylation. Amino group on the pyridine ring was identified as the main reactive site, which was further confirmed by DFT calculation. It was susceptible attacked by SO4 center dot- to form deamination, nitration, and self-coupling products. These couples could be further oxidatively dehydrated to form azo and a series of azo derivatives. EOCSAR program predicted significant hazards on aquatic species during the formation of these couplings and azo derivatives. Our work emphasized the potential ability and toxicity of contaminates to produce azo substances in the presence of amino groups on the pyridine ring.