Methyl group geometries, C–H bond properties and internal rotation in dicarbonyl(η5-cyclopentadienyl)methyl-iron(II) and -ruthenium(II), [MMe(η5-C5H5)(CO)2](M = Fe or Ru)

Abstract
Vibrational spectra have been recorded for the CH3, CD3 and CHD2 isotopomers of [MMe(cp)(CO)2](M = Fe or Ru; cp = cyclopentadienyl). The effects of Fermi resonance were considered in detail and the resonance-corrected CH and CD stretching frequencies used to predict methyl group geometries. Only one ‘isolated’ CH stretching absorption, νisCH, is observed in each CHD2 isotopomer. The results are not consistent with a model in which the methyl groups are subject to an effective barrier to internal rotation, with significant variation of CH bond length with orientation. The spectra are best interpreted in terms of an essentially freely rotating methyl group in which the individual CH bonds undergo a small variation in bond length with rotational angle. The larger barriers which occur in the tricarbonyl compounds [MMe(cp)(CO)3](M = Cr, Mo or W) are likely to be primarily steric in origin, whereas that in [TiMe(cp)Cl2] may arise from an interaction between a CH bonding pair and an unoccupied titanium orbital. The Ru–CH3 bond appears to be slightly weaker than the Fe–CH3 bond, in contrast with results for earlier groups in the d block, in which M–CH3 bond strengths increase down each group.

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