Synthesis and isomerisation of two metallated N,O-complexes of ruthenium: Models for the Murai reaction

Reference:

Jazzar, R. F. R., Varrone, M., Burrows, A. D., Macgregor, S. A., Mahon, M. F. and Whittlesey, M. K., 2006. Synthesis and isomerisation of two metallated N,O-complexes of ruthenium: Models for the Murai reaction. Inorganica Chimica Acta, 359 (3), pp. 815-820.

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Abstract

Two isomers of the N,O-coordinated acetylpyrrolyl complex [Ru(PPh3)(2)(Co)(NC4H3C(O)CH3)H] {cis-NH (1) and trans-NH (2) have been prepared as models for catalytic intermediates in the Murai reaction. Complex 2 isomerises to I upon heating via a dissociative pathway (Delta H++ = 195 +/- 41 kJ mol(-1); Delta S++ = 232 +/- 62 J mol(-1) K-1); the mechanism of this process has been modeled using density functional calculations. Complex 2 displays moderate catalytic activity for the Murai coupling of 2'-methylacetophenone with trimethylvinylsilane, but 1 proved to be catalytically inactive under the same conditions. (c) 2005 Elsevier B.V. All rights reserved.

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