Abstract
Treatment of Cr(NO)(NiPr2)3 with 2 equiv of PhCO2H affords Cr(NO)(NiPr2)(O2CPh)2 (1) in good yields. Reaction of CpNa·DME with 1 produces CpCr(NO)(NiPr2)(OC(O)Ph) (2), which subsequently yields a series of 18-valence-electron (18e) complexes, CpCr(NO)(NiPr2)(R) (R = η1-Cp (3), CH2SiMe3 (4), η1-CH2Ph (5), Ph (6), CPhCH2 (7), C⋮CCMe3 (8), C⋮CPh (9)) when treated with additional CpNa·DME or 1 equiv of the appropriate R2Mg·x(dioxane) reagent. 2−9 are low-spin (S = 0) compounds, and their electronic stability is attributed to the strong, synergic π-bonding interactions present in the [Cr(NO)(NiPr2)]2+ core, as indicated both by the NMR and IR spectra of these complexes and by the solid-state molecular structures of 2−4. The “strong-field” nitrosyl and amide ligands also enforce a diamagnetic configuration on the 14e bis(hydrocarbyl) complexes Cr(NO)(NiPr2)R2 (R = CH2SiMe3 (10), CH2Ph (11), o-tolyl (12)), which are obtained in good yields by reaction of 1 with 2 equiv of the corresponding R2Mg·x(dioxane) reacta...
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