Zinc(II) phthalocyanines immobilized in mesoporous silica Al-MCM-41 and their applications in photocatalytic degradation of pesticides.
Zinc(II) phthalocyanines immobilized in mesoporous silica Al-MCM-41 and their applications in photocatalytic degradation of pesticides.
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DOI：
10.1016/j.jhazmat.2012.06.059
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发表时间：
2012-09
影响因子：
13.6
通讯作者：
Manuela Ramos Silva;M. Calvete;N.P.F. Goncalves;Hugh D. Burrows;M. Sarakha;Aline Fernandes;Maria Filip
中科院分区：
文献类型：
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作者：
Manuela Ramos Silva;M. Calvete;N.P.F. Goncalves;Hugh D. Burrows;M. Sarakha;Aline Fernandes;Maria Filip
在本研究中，作者研究了三种新的锌(II)酞菁(锌(II)四硝基酞菁(ZnTNPc)，锌(II)四(苯氧基)酞菁(ZnTPhOPc)和四碘盐锌(II)四(N，N，N-三甲氨基乙氧基)邻苯二甲酸锌(ZnTTMAEOPcI))固定在Al-MCM-41中。通过漫反射-紫外-可见光谱(DRS-UV-Vis)、发光、热重分析(TG/DSC)、氮气吸附和元素分析等手段对样品进行了表征。比较研究了这三种体系在320-460 nm波段的光催化降解农药杀灭磷和五氯苯酚的性能。结果表明，活性最高的体系是ZnTNPc@Al-MCM-41和ZnTTMAEOPcI@Al-MCM-41，其中固定化的阳离子酞菁的催化性能最好。该体系在经过三次光催化循环后仍表现出较高的活性。LC-MS产物表征和机理研究表明，这些固定化光敏剂激发产生的单线态氧(1O2)是光催化降解这两种农药的关键中间体。
In the present study the authors investigated a set of three new zinc(II) phthalocyanines (zinc(II) tetranitrophthalocyanine (ZnTNPc), zinc(II) tetra(phenyloxy)phthalocyanine (ZnTPhOPc) and the tetraiodide salt of zinc(II)tetra(N,N,N-trimethylaminoethyloxy) phthalocyaninate (ZnTTMAEOPcI)) immobilized into Al-MCM-41 prepared via ship-in-a-bottle methodology. The samples were fully characterized by diffuse reflectance-UV–vis spectroscopy (DRS-UV–vis), luminescence, thermogravimetric analysis (TG/DSC), N2adsorption techniques and elemental analysis. A comparative study was made on the photocatalytic performance upon irradiation within the wavelength range 320–460nm of these three systems in the degradation of pesticides fenamiphos and pentachlorophenol. ZnTNPc@Al-MCM-41 and ZnTTMAEOPcI@Al-MCM-41 were found to be the most active systems, with the best performance observed with the immobilized cationic phthalocyanine, ZnTTMAEOPcI@Al-MCM-41. This system showed high activity even after three photocatalytic cycles. LC–MS product characterization and mechanistic studies indicate that singlet oxygen (1O2), produced by excitation of these immobilized photosensitizers, is a key intermediate in the photocatalytic degradation of both pesticides.