Journal
ACS CATALYSIS
Volume 4, Issue 9, Pages 3227-3236Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs500796u
Keywords
olefin metathesis; heterogeneous catalysts; mesoporous molecular sieves; catalyst immobilization; ruthenium
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Funding
- Czech Science Foundation [P106/12/0189]
- National Center of Science (NCN)
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Ruthenium olefin metathesis catalysts bearing a polar quaternary ammonium group in N-heterocyclic ligand were immobilized on silica and siliceous mesoporous molecular sieves with different pore sizes (SBA-15 and MCM-41). The activity of the heterogeneous catalysts was found to increase with an increase in pore size of the support used, with the best results observed for SBA-15-supported catalyst. The influence of reaction conditions (temperature, solvent, catalyst, and substrate concentration) on the efficiency of new heterogeneous catalysts was established. A significant influence of the counterion present in the ruthenium complex on the activity of immobilized catalysts was also found: those derived from chloride containing ion exhibited the highest activity. High activity in ring-closing metathesis of substrates as citronellene, 1,7-octadiene, and diallyl compounds as well as in cross-metathesis of unsaturated aliphatic compounds with methyl acrylate was observed under optimized conditions. In some cases, heterogenization led to catalysts with efficiency higher than those observed for corresponding homogeneous complexes.
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