Modification of catalytic activity of complexes of Fe(II,III) acetylacetonates with quaternary ammonium salts in the ethylbenzene oxidation with molecular O2 in the presence of small amounts of H2O

被引:0
作者
Matienko, L. I. [1 ]
Mosolova, L. A. [1 ]
机构
[1] Russian Acad Sci, Emanuel Inst Biochem Phys, Moscow 119991, Russia
来源
OXIDATION COMMUNICATIONS | 2008年 / 31卷 / 02期
关键词
oxidation; ethylbenzene; alpha-phenylethylhydroperoxide; homogeneous catalysis; dioxygen; iron(III) tris(acetylacetonate); quaternary ammonium salts; trace amount of H2O;
D O I
暂无
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The catalytic effects of small amounts of H2O (similar to 10(-3) mol/l), introduced in the ethylbenzene oxidation with molecular O-2 catalysed with {Fe(III)(acac)(3) + R4NBr} systems, where R4NBr = exo ligands-modifiers, quaternary ammonium salts CTAB, (C2H5)(4)NBr, Me4NBr, were discovered by us. The synergetic effects of increase in the selectivity (S-PEH) and the conversion degree (C) (parameter (S) over tilde .C) of ethylbenzene oxidation with molecular O-2 to a-phenylethylhydroperoxide (PEH) were obtained in the case of ethylbenzene oxidation catalysed with {Fe(III)(acac)(3) + CTAB+ H2O} system. The proposed 'dioxygenase-like' mechanism of iron catalyst transformation into new catalytic particles in the course of oxidation process in the presence {Fe(III)(acac)(3)(+) R4NBr} and activating additives of the water is discussed. The method of evaluation of the activity of formed complexes (Fe(II)(acac)(2))(x)(R4NBr)(y)(H2O)(n) in the micro-stages of the catalytic chain-radical ethylbenzene oxidations is offered.
引用
收藏
页码:285 / 299
页数:15
相关论文
共 33 条
[1]  
[Anonymous], PHASE TRANSFER CATAL
[2]  
[Anonymous], 1979, FUNDAM RES HOMOGENEO
[3]   Kinetics and mechanism of the Cu(I) and Cu(II) flavonolate-catalyzed oxygenation of flavonol.: Functional quercetin 2,3-dioxygenase models [J].
Balogh-Hergovich, É ;
Kaizer, J ;
Speier, G .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2000, 159 (02) :215-224
[4]   OXYGEN CARRIER AND REDOX PROPERTIES OF SOME NEUTRAL COBALT CHELATES - AXIAL AND IN-PLANE LIGAND EFFECTS [J].
CARTER, MJ ;
RILLEMA, DP ;
BASOLO, F .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1974, 96 (02) :392-400
[5]   Syntheses, structures, and reactivities of cobalt(III)-alkylperoxo complexes and their role in stoichiometric and catalytic oxidation of hydrocarbons [J].
Chavez, FA ;
Rowland, JM ;
Olmstead, MM ;
Mascharak, PK .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1998, 120 (35) :9015-9027
[6]   Onium-decavanadate ion-pair complexes as catalysts in the oxidation of hydrocarbons by O2 [J].
Csányi, LJ ;
Jáky, K ;
Dombi, G ;
Evanics, F ;
Denö, G ;
Kóta, Z .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 195 (1-2) :101-111
[7]   Investigation of the catalytic behavior of ion-pair complexes of vanadium(V) in the liquid-phase oxidation of hydrocarbons with molecular O2 [J].
Csányi, LJ ;
Jáky, K ;
Galbács, G .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2000, 164 (1-2) :109-124
[8]   The role of onium salts in the oxidation of hydrocarbons by O2 catalysed by cationic phase-transfer reagents [J].
Csányi, LJ ;
Jáky, K ;
Pálinkó, I ;
Rockenbauer, A ;
Korecz, L .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (17) :3801-3805
[9]   Mechanistic studies of two dioxygenases in the methionine salvage pathway of Klebsiella pneumoniae [J].
Dai, Y ;
Pochapsky, TC ;
Abeles, RH .
BIOCHEMISTRY, 2001, 40 (21) :6379-6387
[10]  
Emanuel N.M., 1973, ROLE MEDIUM RADICAL