Abstract
Reactions of the Ru(II) amido complexes TpRuL2(NHPh) (L = CO, PMe3, or P(OMe)3) with AgOTf (OTf = trifluoromethanesulfonate) yield the binuclear complexes [TpRuL2NH(C6H4−)]2[OTf]2 along with the Ru(II) amine complexes [TpRuL2(NH2Ph)][OTf] in an approximate 1:1 molar ratio. In these reactions, the two ruthenium fragments are coupled via C−H bond cleavage and C−C bond formation at the para position of anilido ligands. A resonance structure corresponding to Ru(II) metal centers linked by a diimine ligand contributes significantly to the bonding. Evidence for such a contribution comes from the diamagnetic nature of the binuclear complexes and a solid-state X-ray crystallographic study of [TpRu{P(OMe)3}2NH(C6H4−)]2[OTf]2. It is proposed that the coupled products are formed via initial single-electron oxidation followed by C−C bond formation. Variable-temperature NMR spectra of the aryl-coupled complexes are consistent with two geometrical isomers around the rigid HN−C6H4−C6H4NH bridges.
Published Version
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