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金属氧化物对十氯联苯的降解研究
引用本文:刘莎,石瑞芳,黄学敏,黄林艳,刘烨煊,黎烈武,芦会杰,杨帆,苏贵金.金属氧化物对十氯联苯的降解研究[J].中国科学:化学,2014(10):1665-1674.
作者姓名:刘莎  石瑞芳  黄学敏  黄林艳  刘烨煊  黎烈武  芦会杰  杨帆  苏贵金
作者单位:西北水资源与环境生态教育部重点实验室;西安建筑科技大学环境与市政工程学院;环境化学与生态毒理学国家重点实验室;中国科学院生态环境研究中心;环境化学与生态毒理学国家重点实验室中国科学院生态环境研究中心;澳洲矿业工程咨询公司;
基金项目:中国科学院知识创新工程重要方向项目(KZCX2-YW-QN407);国家高技术研究发展计划(2012AA062803);国家重点基础研究发展计划(2009CB421606);国家自然科学基金项目(21177141,51078346)
摘    要:分别以市售的Fe2O3、MgO和CaO为催化剂,对十氯联苯(CB209)进行了催化降解研究.结果表明,MgO对CB209的降解具有较高的活性.在反应温度为300℃,反应时间为60 min时,MgO对CB209的降解效率达到98.9%.进一步研究表明,MgO催化降解CB209的动力学符合准一级动力学反应.通过GC-MS和GC-ECD,并结合衍生化实验,检测到九氯联苯、五氯苯和四氯苯、五氯苯酚、四氯苯酚和三氯苯酚等降解产物,进而推测出MgO催化降解CB209的过程中存在相互竞争的反应路径:氧化反应、碳碳桥键断裂和加氢脱氯.

关 键 词:金属氧化物  十氯联苯  加氢脱氯  氧化反应  碳碳桥键

Degradation of decachlorobiphenyl using metal oxide
Institution:LIU Sha,SHI RuiFang,HUANG XueMin,HUANG LinYan,LIU YeXuan,LI LieWu,LU HuiJie,YANG Fan,SU GuiJin(1 Key Laboratory of Northwest Water Resource, Environment and Ecology, Ministry of Education; School of Environmental & Municipal Engineering, Xi'an University of Architecture & Technology, Xi'an 710055, China; 2 State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; 3 Ausenco Beijing Limited, Beijing 100200, China)
Abstract:The catalytic activities of commercial Fe2O3, MgO and CaO were evaluated by degradating decachlorobiphenyl(CB209). The results showed that MgO exhibited the highest activity, and the degradation efficiency of CB209 over MgO reached 98.9% at 300 °C for 60 min. Furthermore, the result on reaction kinetics study indicates the decomposition of CB209 over MgO conformed to pseudo first order kinetics. Several intermediate products, including nonachlorobiphenyl, pentachlorobenzene, tetrachlorobenzene, pentachlorophenol, tetrachlorophenol and trichlorophenyl, were identified by GC-MS, GC-ECD and derivatization experiment. These products indicate three degradation pathways of CB209, hydrodechlorination, the breakage of C–C bridge bond and oxidative reaction, which are competitively occurring over MgO.
Keywords:metal oxide  decachlorobiphenyl  hydrodechlorination  oxidative reaction  the breakage of C–C bridge bond
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