Journal
CHEMCATCHEM
Volume 5, Issue 8, Pages 2278-2287Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201300021
Keywords
heterogeneous catalysis; mesoporous materials; metathesis; ruthenium; silanes
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Funding
- Natural Science Foundation of China [20903064, 21173137]
- Program for the Top Young Academic Leaders of Higher Learning Institutions of Shanxi [2011002]
- Middle-aged Innovative Talents of Higher Learning Institutions of Shanxi [20120202]
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By postreducing the window size through silylation, 2nd generation Hoveyda-Grubbs catalyst was encapsulated in the nanocages of a mesoporous material SBA-1. The encapsulation efficiency of SBA-1 was up to 70%, much higher than that of other mesoporous materials such as SBA-16, FDU-12, and MCM-41 (0-43 %). The successful encapsulation was confirmed by N-2 sorption analysis and FTIR and diffusion reflectance UV/Vis spectroscopy. Such a SBA-1-encapsulated catalyst showed good activity in both olefin ring-closing metathesis and cross metathesis. A wide range of olefins could be transformed to the desired products with conversions of 27-100 %. The encapsulated catalyst showed more sensitive temperature effects than the homogeneous counterpart, reflecting the unique properties of the encapsulated catalyst. At reaction temperatures of 40-60 degrees C, the activity of the encapsulated catalyst was sufficiently comparable to that of the homogeneous catalyst for the cross metathesis of styrene-type substrates, probably because of the confinement effects of the nanocages. The solid catalyst could be recycled seven times. This study not only supplies a new solid catalyst for olefin metathesis but also demonstrates our improvement in immobilizing metal complex catalyst toward a green and effective level.
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