Abstract
Tropolone and its N-derivatives isopropylaminotropone and diisopropylaminotroponimine react with [Cp*Ru(CH3CN)3]PF6 as the source of the electron-rich Cp*Ru+ synthon in a simple “capping reaction” to the first cyclopentadienyl/cycloheptatrienyl sandwich complexes containing two vicinal oxo or amino substituents. These heteroleptic, cationic C5/C7 π-complexes, [Cp*Ru(C7H5)O2H]+ (4), [Cp*Ru(C7H5)O(NiPr)H]+ (5), and [Cp*Ru(C7H5)(NiPr)2H]+ (6), are air-stable 18-electron metallocenes without precedence. In solution, NMR spectroscopy proves the principal π-coordination of the substituted η7-cycloheptatrienyl ligands, whereas in the solid state a η5-cycloheptatrienyl coordination mode with bent oxo/imino moieties prevails, as shown by X-ray single-crystal structure analyses. Chemically, these compounds are the conjugate Bronsted acids of neutral [O,O]-, [N,O]-, or [N,N]-metalloligands. Reaction with metal acetates or acetylacetonates by in situ deprotonation and complex formation gives access to trimetallic (M ...
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