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The titanocene complexes Cp' 2 Ti(η 2 -Me 3 SiC 2 SiMe 3 ) (Cp' = Cp ( 1 ), Cp* ( 2 )) react with pyrrole under the formation of the titanium(III) mono- N -pyrrolides Cp' 2 Ti(NC 4 H 4 ) (Cp' = Cp ( 6 ), Cp* ( 7 )); whereas the corresponding zirconocene system Cp 2 Zr(η 2 -Me 3 SiC 2 SiMe 3 )(thf) ( 3 ) forms in a different reaction pathway first the Cp 2 Zr(NC 4 H 4 )[C(SiMe 3 )=CH(SiMe 3 )] ( 8 ) and then the zirconium(IV) bis- N -pyrrolide Cp 2 Zr(NC 4 H 4 ) 2 ( 11 ). With Cp* 2 Zr(η 2 -Me 3 SiC 2 SiMe 3 ) ( 4 ) and pyrrole, the zirconium(IV) mono- N -pyrrolide with an agostic alkenyl group Cp* 2 Zr(NC 4 H 4 )[C(SiMe 3 )=CH(SiMe 3 )] ( 9 ) was obtained. In the reaction of the ethylenebistetrahydroindenyl (ebthi) complex rac -(ebthi)Zr(η 2 -Me 3 SiC 2 SiMe 3 ) ( 5 ) with 2,3,5,6-tetrafluoroaniline under N-H bond activation, a complex with an agostic alkenyl group rac -(ebthi)Zr(NH-C 6 HF 4 )[C(SiMe 3 )=CH(SiMe 3 )] ( 10 ) was formed. Compound 10 reacts with additional 2,3,5,6-tetrafluoroaniline to give the bisanilide rac -(ebthi)Zr(NH-C 6 HF 4 ) 2 ( 12 ) which was obtained directly from 5 with two equivalents of 2,3,5,6-tetrafluoroaniline. In reactions of complex 5 with unsubstituted aniline to rac -(ebthi)Zr(NH-C 6 H 5 ) 2 ( 13 ) and with pentafluorophenol to bisphenolate rac -(ebthi)Zr(O-C 6 F 5 ) 2 ( 14 ), no intermediates could be isolated. The new reaction products 6 , 9 , 10 , 12 , 13 and 14 were investigated by X-ray crystallography.

Reactions of Titanocene- and Zirconocene-Bis(trimethylsilyl)acetylene Complexes with Selected Heterocyclic and Aromatic NH and OH Acid Compounds