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| 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. [email protected]
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| 发表期刊 | APPLIED CLAY SCIENCE
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| ISSN | 0169-1317 |
| 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 |
| DOI | 10.1016/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 | |
| 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. [email protected] |
| 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 |
| 推荐引用方式 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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