Ru complexes of Hoveyda-Grubbs type immobilized on lamellar zeolites: activity in olefin metathesis reactions

被引:21
作者
Balcar, Hynek [1 ]
Zilkova, Nadezda [1 ]
Kubu, Martin [1 ]
Mazur, Michal [1 ]
Bastl, Zdenek [1 ]
Cejka, Jiri [1 ]
机构
[1] Acad Sci Czech Republ, Vvi Dolejskova 2155 3, J Heyrovsky Inst Phys Chem, CR-18223 Prague 8, Czech Republic
关键词
Hoveyda-Grubbs type catalyst; hybrid catalysts; lamellar zeolites; non-covalent immobilization; olefin metathesis; MESOPOROUS MOLECULAR-SIEVES; RUTHENIUM CARBENES; CATALYSTS; SILICA; STRATEGIES;
D O I
10.3762/bjoc.11.225
中图分类号
O62 [有机化学];
学科分类号
070303 ; 081704 ;
摘要
Hoveyda-Grubbs type catalysts with cationic tags on NHC ligands were linker-free immobilized on the surface of lamellar zeolitic supports (MCM-22, MCM-56, MCM-36) and on mesoporous molecular sieves SBA-15. The activity of prepared hybrid catalysts was tested in olefin metathesis reactions: the activity in ring-closing metathesis of citronellene and N,N-diallyltrifluoroacetamide decreased in the order of support MCM-22 approximate to MCM-56 > SBA-15 > MCM-36; the hybrid catalyst based on SBA-15 was found the most active in self-metathesis of methyl oleate. All catalysts were reusable and exhibited low Ru leaching (< 1% of Ru content). XPS analysis revealed that during immobilization ion exchange between Hoveyda-Grubbs type catalyst and zeolitic support occurred in the case of Cl- counter anion; in contrast, PF6- counter anion underwent partial decomposition.
引用
收藏
页码:2087 / 2096
页数:10
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