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Synthesis and small molecule reactivity of trans-dihydride isomers of Ru(NHC)2(PPh3)2H2 (NHC = N-Heterocyclic Carbene)


Reference:

Davies, C. J. E., Lowe, J. P., Mahon, M. F., Poulten, R. C. and Whittlesey, M. K., 2013. Synthesis and small molecule reactivity of trans-dihydride isomers of Ru(NHC)2(PPh3)2H2 (NHC = N-Heterocyclic Carbene). Organometallics, 32 (17), pp. 4927-4937.

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http://dx.doi.org/10.1021/om400648x

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Abstract

Addition of IMe4 (1,3,4,5-tetramethylimidazol-2-ylidene) to Ru(PPh3)3HCl (in the presence of H2) or Ru(PPh3)4H2 gave the all-trans isomer of Ru(IMe4)2(PPh3)2H2 (1a), whereas 1,3-diethyl-4,5-dimethylimidazol-2-ylidene (IEt2Me 2) reacted with Ru(PPh3)4H2 to form cis,cis,trans-Ru(IEt2Me2)2(PPh 3)2H2 (2b). H/D exchange of 1a with C 6D6 (elevated temperature) or D2 (room temperature) gave Ru(IMe4)2(PPh3)2HD (1a-HD) and Ru(IMe4)2(PPh3)2D 2 (1a-D2). CO reacted with 1a to give a mixture of Ru(IMe4)2(PPh3)(CO)H2 (3) and Ru(IMe4)2(CO)3 (4); 2b reacted in a similar manner, although more slowly, allowing isolation of the monocarbonyl species Ru(IEt2Me2)2(PPh3)(CO)H2 (5). Insertion of CO2 into one of the Ru-H bonds of 1a and 2b generated mixtures of major and minor isomers of the κ2-formate complexes Ru(IMe4)2(PPh3)(OCHO)H (7/8) and Ru(IEt2Me2)2(PPh3)(OCHO)H (9/10). The hydridic nature of 1a and 2b was apparent by their reactivity toward MeI, which gave [Ru(IMe4)2(PPh3)2H]I (11), Ru(IEt2Me2)2(PPh3)HI (12), [Ru(IEt2Me2)2(PPh3)2H]I (13), and Ru(IEt2Me2)(PPh3)2HI (14). Complexes 1a, 2b, 5, 9, 11, 13, and 14 were structurally characterized.

Details

Item Type Articles
CreatorsDavies, C. J. E., Lowe, J. P., Mahon, M. F., Poulten, R. C. and Whittlesey, M. K.
DOI10.1021/om400648x
Related URLs
URLURL Type
http://www.scopus.com/inward/record.url?scp=84883789741&partnerID=8YFLogxKUNSPECIFIED
DepartmentsFaculty of Science > Chemistry
Research CentresCentre for Sustainable Chemical Technologies
RefereedYes
StatusPublished
ID Code37251

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