Abstract
Treatment of the TpRu complex Tp(PPh3)2RuCl (Tp = HB(pz)3, pz = pyrazolyl) (1) with ethynylferrocene in MeOH gave the trimetallic alkenyl ketone complex Tp(PPh3)Ru{C(Fc) = CHC(O)CH2(Fc)} (Fc=(η5-C5H4)Fe(η5-C5H5)) (2). Intriguingly, a similar reaction was performed in the presence of NaOMe afforded the dimetallic acetylide complex Tp(PPh3)2Ru–CC-Fc (3). A number of new cationic vinylidene complexes [Tp(PPh3)2Ru{ = CC(Fc)CH2R}]+ [4a, R = CN; 4b, R = HCCH2; 4c, R = CHC(CH3)2; 4d, R = Ph] have been prepared by electrophilic addition of organic halides to complex 3. The substitution reaction of 4a with pyrazole is followed by an intramolecular nucleophilic addition of the nitrogen atom at the α-carbon atom and removal of HI to afford the metallacyclic complex, Tp(PPh3)Ru(C3H3NN)CC(Fc) CH2CN (5a). All of the complexes are identified by spectroscopic methods as well as elementary analysis. The structure of 2 has been determined by X-ray diffraction analysis. Pathways for the synthesis of these compounds are proposed.
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