Immobilization of multifunctional Schiff base containing ruthenium complexes on MCM-41

被引:98
作者
De Clercq, B
Lefebvre, F
Verpoort, F
机构
[1] Univ Ghent, Div Organomet Chem & Catalysis, Dept Inorgan & Phys Chem, B-9000 Ghent, Belgium
[2] CNRS, UMR CPE 9986, Lab LCOMS, F-69616 Villeurbanne, France
关键词
heterogeneous catalysis; olefin metathesis; Kharasch addition; atom transfer radical polymerization; vinylation;
D O I
10.1016/S0926-860X(03)00126-1
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
Two solid catalysts in which a Schiff base containing ruthenium complex has been covalently anchored on MCM-41 have been prepared and characterized. The catalytic behavior of these materials in ring-closing metathesis (RCM), ring-opening metathesis polymerization (ROMP), Kharasch addition, atom transfer radical polymerization (ATRP) and vinylation reactions as well as the recycling characteristics in RCM reactions are presented to exemplify the effectiveness and the multifunctional character of these catalytic systems. For ROMP the influence of the polymerization solvent on the performance of the catalysts was checked. For the RCM reactions both reaction time and reaction temperature were varied in order to determine the influence of these parameters on the RCM activity of our catalysts. The activity of our catalytic systems in radical reactions such as ATRP and the Kharasch addition is promising. Our results demonstrate that the ATRP process of styrene proceeds in a controlled fashion allowing the synthesis of well-defined polymers. Furthermore, we were able to demonstrate that the Kharasch activity of our catalysts shows a pronounced temperature dependence. In addition to all this, we also postulated a mechanism that explains for the observed selectivities in the vinylation experiments. The host-guest interaction of these hybrid catalytic systems is studied by XRD, XRF, ICP/MS, BET, FT-Raman and solid state NMR analysis. (C) 2003 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:345 / 364
页数:20
相关论文
共 48 条
[1]  
Abbenhuis HCL, 1999, ANGEW CHEM INT EDIT, V38, P1058, DOI 10.1002/(SICI)1521-3773(19990419)38:8<1058::AID-ANIE1058>3.0.CO
[2]  
2-8
[3]   A recyclable 'boomerang' polymer-supported ruthenium catalyst for olefin metathesis [J].
Ahmed, M ;
Barrett, AGM ;
Braddock, DC ;
Cramp, SM ;
Procopiou, PA .
TETRAHEDRON LETTERS, 1999, 40 (49) :8657-8662
[4]   Metal vinylidenes in catalysis [J].
Bruneau, C ;
Dixneuf, PH .
ACCOUNTS OF CHEMICAL RESEARCH, 1999, 32 (04) :311-323
[5]  
BUCHMEISER MR, 2002, NATO ADV STUDY I ASI, P195
[6]   Heterogeneous catalysis in liquid phase transformations of importance in the industrial preparation of fine chemicals [J].
Clark, JH ;
Macquarrie, DJ .
ORGANIC PROCESS RESEARCH & DEVELOPMENT, 1997, 1 (02) :149-162
[7]   Environmentally friendly catalytic methods [J].
Clark, JH ;
Macquarrie, DJ .
CHEMICAL SOCIETY REVIEWS, 1996, 25 (05) :303-&
[8]  
CORNILS B, 2000, CATALYSIS A Z CONCIS
[9]  
Crabtree R.H., 1988, ORGANOMETALLIC CHEM
[10]   Oxidation of benzyl alcohol using polymer anchored Ru(III) complex as catalyst [J].
Dalal, MK ;
Upadhyay, MJ ;
Ram, RN .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1999, 142 (03) :325-332