Efficient photodegradation of 2,4-dichlorophenol in aqueous solution catalyzed by polydivinylbenzene-supported zinc phthalocyanine

Efficient photodegradation of 2,4-dichlorophenol in aqueous solution catalyzed by polydivinylbenzene-supported zinc phthalocyanine
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聚二乙烯基苯负载锌酞菁催化高效光降解水溶液中2,4-二氯苯酚

DOI:
10.1016/j.molcata.2007.01.022
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发表时间:
2007-05
影响因子:
--
通讯作者:
Xu, Shirong
Xu, Shirong
中科院分区:
化学2区
文献类型:
--
作者:
Wu, Lin;Zhang, Quanxing;Gao, Gu;ao;Fei, Zhenghao;Li, Aimin;Xu, Shirong

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本文研究了以氯甲基化聚二乙烯基苯和锌酞菁为原料,经Friedel-Craft反应制得的聚二乙烯基苯负载锌酞菁(PDVB-ZnPc)光催化降解2,4-二氯苯酚(2,4-DCP)的反应。用气相色谱-质谱法(GC-MS)对反应中间产物进行了鉴定。用电子顺磁共振(EPR)技术确定了反应中涉及的活性氧物种。实验结果表明,PDVB-ZnPc对水溶液中有毒的2,4-DCP有较好的去除和矿化作用。辐照4h后,脱色率可达98%。该反应符合准一级反应动力学,符合Langmuir-HinShelwood方程。反应的最适浓度为1.0g/L,反应中间产物为可生物降解的有机酸,在碱性条件下可矿化为CO32-−和Cl-−。在我们的反应体系中,2,4-DCP的光降解过程中可能产生了羟基自由基和超氧阴离子自由基,而不是单线态氧。
In this study, photodegradation of 2,4-dichlorophenol (2,4-DCP) in aerated aqueous solution at pH 13 in the presence of hydrogen peroxide catalyzed by polydivinylbenzene-supported zinc phthalocyanine (PDVB-ZnPc) prepared from chloromethylated polydivinylbenzene and zinc phthalocyanine via a Friedel–Crafts reaction has been investigated. The reaction intermediates were identified by gas chromatography–mass spectrometry (GC–MS). The reactive oxygen species involved in the reaction were determined by electron paramagnetic resonance (EPR) technique. Based on the experimental results obtained, PDVB-ZnPc was found to be effective for removing and mineralizing the toxic 2,4-DCP in aqueous solution. The removal yield amounted to 98% after 4h of irradiation. The reaction followed pseudo-first-order kinetics, and was well fitted into the Langmuir–Hinshelwood-type equation. The optimal concentration of PDVB-ZnPc was 1.0g/l. The reaction intermediates were some biodegradable organic acids which were subsequently mineralized to CO32−and Cl−in alkaline solution. Hydroxyl radical and superoxide anion radical other than singlet oxygen were probably generated during the photodegradation of 2,4-DCP in our reaction system.
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