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Zinc(II) phthalocyanines immobilized in mesoporous silica Al-MCM-41 and their applications in photocatalytic degradation of pesticides

机译:固定在介孔二氧化硅Al-MCM-41中的锌(II)酞菁及其在农药的光催化降解中的应用

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摘要

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), N2 adsorption techniques and elemental analysis. A comparative study was made on the photocatalytic performance upon irradiation within the wavelength range 320–460 nm 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.
机译:在本研究中,作者研究了一组三种新的锌(II)酞菁锌(锌(II)四硝基酞菁(ZnTNPc),锌(II)四(苯氧基)酞菁(ZnTPhOPc)和锌(II)tetra(四(将N,N,N-三甲基氨基乙氧基)酞菁酸酯(ZnTTMAEOPcI)固定到通过瓶装船方法制备的Al-MCM-41中。样品通过漫反射-紫外-可见光谱(DRS-UV-vis),发光,热重分析(TG / DSC),N2吸附技术和元素分析进行​​了全面表征。在这三个系统的波长范围为320–460 nm的辐照下,对农药fenamiphos和五氯苯酚的降解具有光催化性能进行了比较研究。 ZnTNPc @ Al-MCM-41和ZnTTMAEOPcI @ Al-MCM-41被发现是最活跃的系统,在固定化的阳离子酞菁ZnTTMAEOPcI @ Al-MCM-41上观察到的性能最佳。即使经过三个光催化循环,该系统仍显示出高活性。 LC-MS产品的表征和机理研究表明,通过激发这些固定的光敏剂而产生的单线态氧(1O2)是两种农药光催化降解的关键中间体。

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