Synthesis And Characterization Of Symmetrical And Unsymmertical Metal Phthalocyanine Complexes In Molecular Sieves

This thesis mainly investigated the feasibility of encapsulation of MPc into the supercages of zeolite Y and the synthesis of unsymmetrical phthalocyanine and its immobilization in MCM-41 and zeolite Y . The catalytic performance of all samples was tested by cyclohexane oxidation as a model reaction.1 , It will be reported of the synthesis of metal phthalocyanine into the supercages of zeolite Y using Phthalic anhydride-Urea route via "ship-in-the-bottle" method , and its characterization by XRIX FT-IR> DRS, TG-DTA etc. The results showed that the synthesis route was feasible and metal phthalocyanine was successfully encapsulated into zeolite Y . The factors affacting the preparation of MPcY were investigated, too .The results manifested that (1) the center ion of Mn2+ was better than Co2+ and Fe 2+ . With increasing the content of the center ion in samples , the cyclohexane conversion increases, but the turnover number (TON) decreases .(2) the optimum reaction condition for preparation of CoPcY is as follows: a , using CoCl2 as the exchanged salt ; b , complexation temperature of 180 ; c . complexation catalyst of NH4C1 and A1C13 .2, The unsymmetrically substituted cobalt phthalocyanine complexes (CoPcBrx) were synthesized by statistical condensation of phthalic anhydride and tetrabromophthalic anhydride, and further immobilized in MCM-41 molecular sieves by zeolite synthesis method, as well as characterized by XRD,FT-IR,DRS, 1HNMRetc. The catalytic property of CoPcBrx/MCM-41was tested by cyclohexane oxidation using H2O2 or t-BOOH as oxidant. The catalytic results showed that the catalytic activity of CoPcBrx/MCM-41 was higher than that of CoPc/MCM-41 and CoPcBri6/MCM-41.3, CoPcBrx Y was prepared by zeolite synthesis method. Moreover , the influences of the factors, e.g. reaction temperature , reaction time , reaction medium , catalyst concentration and the volume ratio of cyclohexane to H2O2, on the catalytic performance in cyclohexane oxidation were also explored. The catalyst results showed : a , With increasing the reaction temperature, the cyclohexane conversion increases . b , in the catalyst concentration, the cyclohexane conversion also enhances, c , acetic acid is the best reaction medium , while acetonitrile was the worst . d , With increasing the amount of H2O2 in reaction system , the higher cyclohexane conversion and the ratio of cyclohexanone to cyclohenanol are obtained . e ,With increasing the reaction time , the conversion of cyclohexane increased and the yeild of cyclohexanone also improves . Moreover , the catalytic activity of the catalyst remains the same after three recycles of reaction under the identical condtion.