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Iron-porphyrin encapsulated in poly(methacrylic acid) and mesoporous Al-MCM-41 as catalysts in the oxidation of benzene to phenol

机译:聚甲基丙烯酸和中孔Al-MCM-41中包裹的铁卟啉作为苯氧化为苯酚的催化剂

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摘要

Poly(methacrylic acid) (PMAA) and mesoporous molecular sieve Al-MCM-41 with Si/Al = 20 were used as supports for the encapsulationudof bulky iron(III)-5,10,15,20-tetra-(4-pyridyl)porphyrin (Fe-TPyP). Metalloporphyrin of Fe(III) was encapsulated inside the mesopores of Al-udMCM-41 by a process of sequential synthesis of Fe-TPyP by treatment of FeCl3 with 5,10,15,20-tetra-(4-pyridyl) porphyrin (TPyP), followedudby encapsulation of Fe-TPyP. Fe-TPyP complexes were also successfully encapsulated in PMAA by polymerizing a monomer (MAA)udwith a cross-linker around the Fe-TPyP complexes. The materials obtained were identified using XRD, UV–vis DR, FTIR and luminescenceudspectroscopies. The oxidation of benzene to phenol using aqueous hydrogen peroxide has been studied using both iron-porphyrin encapsulatedudin poly(methacrylic acid) and mesoporous Al-MCM-41 as catalysts. The encapsulated iron-porphyrin in PMAA (Fe-TPyP–PMAA) give audhigher catalytic activity compared to Fe-TPyP encapsulated in Al-MCM-41 (Fe-TPyP–MCM-41). However, the product selectivity and theudregenerability of Fe-TPyP–PMAA are not as good as than those of Fe-TPyP–MCM-41. One considers that the hydrophobic nature of Fe-udTPyP–PMAA may account for the high catalytic activity, and the ordered structure of Fe-TPyP–MCM-41 may contribute to a high selectivity.ud© 2005 Elsevier B.V. All rights reserved.
机译:聚甲基丙烯酸(PMAA)和Si / Al = 20的介孔分子筛Al-MCM-41被用作载体,包裹大块铁(III)-5、10、15、20-四-(4 -吡啶基)卟啉(Fe-TPyP)。通过用5,10,15,20-四-(4-吡啶基)卟啉处理FeCl3依次合成Fe-TPyP的过程,将Fe(III)的金属卟啉封装在Al- udMCM-41的中孔内( TPyP),然后包裹Fe-TPyP。通过在Fe-TPyP复合物周围用交联剂聚合单体(MAA) ud,Fe-TPyP复合物也成功封装在PMAA中。使用XRD,UV-DR,FTIR和发光/超光谱法鉴定获得的材料。已经研究了使用过氧化氢水溶液将苯氧化为苯酚,同时使用铁卟啉包封的 udin聚(甲基丙烯酸)和中孔Al-MCM-41作为催化剂。与封装在Al-MCM-41(Fe-TPyP“ MCM-41)中的Fe-TPyP相比,PMAA(Fe-TPyP” PMAA)中的铁卟啉封装的催化活性更高。但是,Fe-TPyP – PMAA的产物选择性和还原性不如Fe-TPyP – MCM-41。人们认为Fe- udTPyP– PMAA的疏水性可能解释了高催化活性,而Fe-TPyP– MCM-41的有序结构可能有助于高选择性。 ud©2005 Elsevier BV版权所有保留。

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