Encapsulation of Fe(III) and Cu(II) complexes in NaY zeolite

被引:29
作者
Drechsel, SA [1 ]
Kaminski, RCK [1 ]
Nakagaki, S [1 ]
Wypych, F [1 ]
机构
[1] Univ Fed Parana, Dept Quim, BR-81531990 Curitiba, Parana, Brazil
关键词
NaY zeolite; iron complexes; copper complexes; encapsulation; immobilized complexes;
D O I
10.1016/j.jcis.2004.04.015
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The use of nonporphyrin complexes encapsulated in zeolites as catalysts for oxidation reactions has been improved in the past decades by the discovery of increasing numbers of nonheme monoxygenases. The zeolite lattice can change the oxidative chemistry of the metallocomplexes, resulting in a catalytic effect different from those observed in homogeneous reactions. We report the encapsulation of iron and copper metallocomplexes with the ligand (2-hydroxybenzyl)(2-methylpyridyl)amine, Hbpa, and iron complexes with the ligand N,N'-bis(2-hydroxybenzyl)-N, N'-bis(2-methylpyridyl) ethylenediamine, H(2)bbpen. The zeolite-encapsulated metallocomplexes were prepared by diffusion of the ligands through the pores of the zeolites, already exchanged with the respective metal. The syntheses were performed in methanol and toluene solutions. Elemental analysis of solids with the Hbpa ligand have indicated better complexation for synthesis in toluene, where 74% of the iron atoms were coordinated by the ligand, against 37% for the synthesis in methanol. For the immobilization with the H(2)bbpen ligand in toluene it was observed that 46% of the iron atoms are coordinated, showing that the diffusion of the small ligand Hbpa through the zeolite cage was facilitated. The EPR spectra of the solids show signals at g = 2.0, which was attributed to an Fe-Fe interaction from the noncoordinated atoms, and g = 4.3 attributed to iron (III) in a rhombic geometry. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:138 / 145
页数:8
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