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均相Co/PMS系统降解吡虫啉的影响因素及降解途径研究
摘要点击 2770  全文点击 1638  投稿时间:2007-01-12  修订日期:2007-03-07
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中文关键词  高级氧化技术(AOTs)  硫酸自由基  无机离子  降解机理  废水处理  吡虫啉
英文关键词  advanced oxidation technologies (AOTs)  sulfate radical  inorganic ion  degradation mechanism  wastewater treatment  Imidacloprid
作者单位
陈晓旸 大连理工大学环境科学与工程系大连116024 
陈晓 浙江省农科院环境资源与土壤肥料研究所杭州310021 
陈景文 大连理工大学环境科学与工程系大连116024 
杨萍 大连理工大学环境科学与工程系大连116024 
乔显亮 大连理工大学环境科学与工程系大连116024 
中文摘要
      过渡态Co2+-催化分解KHSO5(Co/PMS)系统是一种新型的高级氧化技术,其反应体系可以产生强氧化性的硫酸自由基(SO·-4).以杀虫剂吡虫啉为目标污染物,重点研究了溶液中PMS浓度、Co2+-浓度和无机阴离子(H2PO-4、HCO-3、NO-3和Cl-)对Co/PMS系统降解吡虫啉的影响.结果表明,吡虫啉的降解遵循准一级动力学,其降解速率与氧化剂PMS浓度和催化剂Co2+-的浓度呈正相关.吡虫啉的降解速率随着PMS和Co2+-浓度的增加而增大,但是当PMS与吡虫啉的摩尔比大于20时,增加PMS的浓度对吡虫啉的降解速率反而有一定程度的抑制.H2PO-4能促进Co/PMS系统对虫啉的降解;低浓度的HCO-3促进吡虫啉的降解,高浓度则为抑制作用;Cl-抑制吡虫啉的降解,而NO-3则对整个降解过程影响不明显.研究中采用GC/MS分析吡虫啉降解的中间产物,得到了6-氯烟酸和6-氯烟酰胺2种主要的中间产物,并由此推测其可能的降解途径.
英文摘要
      Cobaltous-mediated decomposition of peroxymonosulfate (Co/PMS) system is one of novel advanced oxidation technologies (AOTs), which leads to the formation of very strong oxidizing species in aqueous phase. Effects of PMS concentrations, Co2+- concentrations and various inorganic anions (H2PO-4, HCO-3, NO-3, Cl-) on the degradation of Imidacloprid induced by Co/PMS system was investigated as emphasis. The degradation kinetics of imidacloprid followed pseudo first-order kinetics and reaction rates related to PMS and Co2+- concentrations. The reaction rates increased with increasing [PMS] and [Co2+-] when the other parameters were constant. However, the decrease of degradation rates was found when the molar ratio of PMS versus imidacloprid was over 20. The effects of H2PO-4 had positive effect on the degradation of Imidacloprid, low concentration HCO-3 had positive effect and high concentration HCO-3 had negative effect, Cl- had negative effect, while NO-3 had little effect. Based on the results of GC/MS, two main intermediates were identified, 6-chloronicotinic acid and 6-chloronicotinamide, and the reaction pathway for SO·-4 induced by homogeneous Co/PMS was proposed accordingly.

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