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题名: Thermal dechlorination of PCB-209 over Ca species-doped Fe2O3
作者: Su, Guijin; Huang, Linyan; Shi, Ruifang; Liu, Yexuan; Lu, Huijie; Zhao, Yuyang; Yang, Fan; Gao, Lirong; Zheng, Minghui
刊名: CHEMOSPHERE
出版日期: 2016-02
卷号: 144, 期号:0, 页码:81-90
关键词: Ca species-doped Fe2O3 ; Polychlorinated biphenyls ; Hydrodechlorination ; Steric effect
DOI: 10.1016/j.chemosphere.2015.08.022
部门归属: 环境化学与生态毒理学国家重点实验室
英文摘要: Degradation reaction of decachlorobiphenyl (PCB-209) was investigated over the synthesized Ca speciesdoped Fe2O3 at 300 degrees C. The 1%Ca-Fe2O3 exhibited the highest activity among the four catalysts prepared with the pseudo-first order reaction at k(obs) = 0.103 min(-1). PCB-207, PCB-197, PCB-176, PCB-184, PCB-150, PCB-136, PCB-148, PCB-104, PCB-96, PCB-54, PCB-19, PCB-4 and PCB-1 were identified as the dominant isomers in their respective nonachlorobiphenyl (NonaCB) to monochlorobiphenyl (MonoCB) homologue groups. Analysis of the hydrodechlorination products indicated that dechlorination was much more favored on meta-and para-than on ortho-positions. The formation of significantly predominant NonaCB and octachlorobiphenyl (OctaCB) isomers was attributed to lower energy principles and to the 90 degrees dihedral angles of two aromatic rings which prevented the hydrodechlorination at ortho-positions. When the number of chlorine atoms is not more than 7, the steric effect supports the formation of predominant PCB isomers having chlorines at four ortho-positions. During the dechlorination of tetrachlorobiphenyl (TetraCB) formed to generate monochlorobiphenyl (MonoCB) isomers, the chlorine atoms fully substituted at the ortho-positions have to be successively removed, with the first two dechlorinations preferentially occurring at the two different benzene rings. This is dissimilar to that of octachloronaphthalene (PCN-75) in which the hydrodechlorination reaction happened preferentially at ortho-position due to the existence of steric effects. The opposite roles of the steric effect in ortho-position between PCB-209 and PCN-75 might be due to the difference of the pi-conjugated plane caused by the dihedral angle of 90 degrees and 0 degrees of the two aromatic rings.(c) 2015 Elsevier Ltd. All rights reserved.
收录类别: SCI
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内容类型: 期刊论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35964
Appears in Collections:环境化学与生态毒理学国家重点实验室_期刊论文

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