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MCM-41-supported ruthenium carbonyl cluster-derived catalysts for asymmetric hydrogenation reactions

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Title MCM-41-supported ruthenium carbonyl cluster-derived catalysts for asymmetric hydrogenation reactions
 
Creator INDRA, ARINDAM
BASU, SUSMIT
KULKARNI, DHANASHREE G
GOPINATH, CHINNAKONDA S
BHADURI, SUMIT
LAHIRI, GOUTAM KUMAR
 
Subject reaction kinetics
catalysts
hydrogenation
transmission electron microscopy
x-ray photoelectron spectroscopy
 
Description The anionic ruthenium carbonyl cluster [Ru4(μ-H)3(CO)12]− has been ion-paired with (3-chloropropyl)trimethoxysilyl-cinchonidium or sparteinium groups chemically bound to the surfaces of MCM-41 [(MCM-41-)(-O)3SiCH2CH2CH2NR3+Cl−, NR3 = cinchonidine or sparteine]. The resultant materials have been characterized before and after use as hydrogenation catalysts by IR, XPS, and TEM. The molecular identity of the cluster is retained in the fresh catalysts, but under hydrogen pressure (≥30 bar) the carbonyl groups are lost. Ruthenium (0) and a small amount of Ru2+ can be observed on the fresh catalyst by XPS, while the used catalyst shows only Ru(0). TEM micrographs show retention of the MCM structure and no observable aggregation of metal. Under optimal conditions, good (≤75%) and observable (≤30%) enantioselectivities are obtained for the hydrogenations of methyl pyruvate and acetophenone, respectively. The enantioselectivity of the catalyst towards methylpyruvate hydrogenation is retained even with relatively high turnovers. This behavior is in sharp contrast to that of the Chini cluster [Pt12(CO)24]2−, derived analogous catalyst reported earlier by us.
 
Publisher Elsevier
 
Date 2009-03-23T05:14:03Z
2011-11-25T20:13:27Z
2011-12-26T13:08:18Z
2011-12-27T05:56:18Z
2009-03-23T05:14:03Z
2011-11-25T20:13:27Z
2011-12-26T13:08:18Z
2011-12-27T05:56:18Z
2008
 
Type Article
 
Identifier Applied Catalysis A: General 344(1-2), 124-130
0926-860X
http://dx.doi.org/10.1016/j.apcata.2008.04.009
http://hdl.handle.net/10054/1074
http://dspace.library.iitb.ac.in/xmlui/handle/10054/1074
 
Language en