Catalytic wet peroxide oxidation of 4-chlorophenol over Al-Fe-, Al-Cu-, and Al-Fe-Cu-pillared clays: Sensitivity, kinetics and mechanism
Zhou, Shiwei1,2; Zhang, Changbo3; Hu, Xuefeng2; Wang, Yuehua3; Xu, Rui2; Xia, Chuanhai2; Zhang, Hua2; Song, Zhengguo3; Song, ZG (reprint author), Minist Agr, Agroenvironm Protect Inst, Tianjin 300191, Peoples R China. forestman1218@163.com
发表期刊APPLIED CLAY SCIENCE
ISSN0169-1317
2014-06-01
卷号95页码:275-283
关键词Fe Cu-pillared Clays Thermal Structural Evolution 4-chlorophenol Peroxide Oxidation Surface-catalyzed Decomposition
DOI10.1016/j.clay.2014.04.024
产权排序[Zhou, Shiwei] Chinese Acad Sci, Inst Soil Sci, Key Lab Soil Environm & Pollut Remediat, Nanjing 210008, Peoples R China; [Zhou, Shiwei; Hu, Xuefeng; Xu, Rui; Xia, Chuanhai; Zhang, Hua] Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Zone Environm Proc & Ecol Remedia, Yantai 264003, Peoples R China; [Zhang, Changbo; Wang, Yuehua; Song, Zhengguo] Minist Agr, Agroenvironm Protect Inst, Tianjin 300191, Peoples R China
作者部门中科院海岸带环境过程与生态修复重点实验室
英文摘要Al-Fe-, Al-Cu-, and Al-Fe-Cu-PILCs were synthesized, characterized and tested in the catalytic wet peroxide oxidation of 4-chlorophenol (4-CP). An apparent induction period followed by a rapid oxidation was observed during the Fenton-like reaction, and the whole reaction could be modeled well using a Fermi's kinetic equation (R-2 = 0.9938 similar to 0.9993). The generation of hydroxyl radicals (HO center dot) from surface-catalyzed decomposition of H2O2 was the oxidation cause whereas the dissolution of active metals was its result. Accordingly, induction period was the cause of heterogeneous surface activation (catalysis or modification) for more HO center dot formed by decreasing pH. 4-CP oxidation proceeded via 4-chlorocatechol (major) and hydroquinone (minor) pathways, along the formation of main intermediate (5-chloro-1,2,4-benzentriol). Finally besides CO2, H2O and Cl- two main compounds (I and II) formed, where the former was identified as 2,4-dioxopentanedioic acid whereas the latter as ferric-oxalate complex. There were marked structural and active differences between Al-Fe-PILC and Al-Cu-PILC in which compared to the latter, the former possessed higher SSA and activity but its optimal calcination temperature was lower and the induction time was also longer. In addition, compound II accounted for a considerable proportion in Al-Fe-PILC system whereas compound I was almost only component in Al-Cu-PILC system. (C) 2014 Elsevier B.V. All rights reserved.; Al-Fe-, Al-Cu-, and Al-Fe-Cu-PILCs were synthesized, characterized and tested in the catalytic wet peroxide oxidation of 4-chlorophenol (4-CP). An apparent induction period followed by a rapid oxidation was observed during the Fenton-like reaction, and the whole reaction could be modeled well using a Fermi's kinetic equation (R-2 = 0.9938 similar to 0.9993). The generation of hydroxyl radicals (HO center dot) from surface-catalyzed decomposition of H2O2 was the oxidation cause whereas the dissolution of active metals was its result. Accordingly, induction period was the cause of heterogeneous surface activation (catalysis or modification) for more HO center dot formed by decreasing pH. 4-CP oxidation proceeded via 4-chlorocatechol (major) and hydroquinone (minor) pathways, along the formation of main intermediate (5-chloro-1,2,4-benzentriol). Finally besides CO2, H2O and Cl- two main compounds (I and II) formed, where the former was identified as 2,4-dioxopentanedioic acid whereas the latter as ferric-oxalate complex. There were marked structural and active differences between Al-Fe-PILC and Al-Cu-PILC in which compared to the latter, the former possessed higher SSA and activity but its optimal calcination temperature was lower and the induction time was also longer. In addition, compound II accounted for a considerable proportion in Al-Fe-PILC system whereas compound I was almost only component in Al-Cu-PILC system. (C) 2014 Elsevier B.V. All rights reserved.
文章类型Article
资助机构Chemistry ; Materials Science ; Mineralogy
收录类别SCI
语种英语
关键词[WOS]ACID ORANGE 7 ; HYDROGEN-PEROXIDE ; WASTE-WATER ; FERMIS EQUATION ; PHENOL ; DEGRADATION ; IRON ; H2O2 ; CWPO ; DECOMPOSITION
研究领域[WOS]Chemistry ; Materials Science ; Mineralogy
WOS记录号WOS:000338612200036
引用统计
被引频次:55[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.yic.ac.cn/handle/133337/8738
专题中国科学院海岸带环境过程与生态修复重点实验室
海岸带生物学与生物资源利用重点实验室_海岸带生物学与生物资源保护实验室
通讯作者Song, ZG (reprint author), Minist Agr, Agroenvironm Protect Inst, Tianjin 300191, Peoples R China. forestman1218@163.com
作者单位1.Chinese Acad Sci, Inst Soil Sci, Key Lab Soil Environm & Pollut Remediat, Nanjing 210008, Peoples R China
2.Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Zone Environm Proc & Ecol Remedia, Yantai 264003, Peoples R China
3.Minist Agr, Agroenvironm Protect Inst, Tianjin 300191, Peoples R China
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GB/T 7714
Zhou, Shiwei,Zhang, Changbo,Hu, Xuefeng,et al. Catalytic wet peroxide oxidation of 4-chlorophenol over Al-Fe-, Al-Cu-, and Al-Fe-Cu-pillared clays: Sensitivity, kinetics and mechanism[J]. APPLIED CLAY SCIENCE,2014,95:275-283.
APA Zhou, Shiwei.,Zhang, Changbo.,Hu, Xuefeng.,Wang, Yuehua.,Xu, Rui.,...&Song, ZG .(2014).Catalytic wet peroxide oxidation of 4-chlorophenol over Al-Fe-, Al-Cu-, and Al-Fe-Cu-pillared clays: Sensitivity, kinetics and mechanism.APPLIED CLAY SCIENCE,95,275-283.
MLA Zhou, Shiwei,et al."Catalytic wet peroxide oxidation of 4-chlorophenol over Al-Fe-, Al-Cu-, and Al-Fe-Cu-pillared clays: Sensitivity, kinetics and mechanism".APPLIED CLAY SCIENCE 95(2014):275-283.
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