Unstable CpNi(vinyl) compounds of the type CpNi-CR'= CR(2) (R' = CH3,
C6H5, R = CH3) are formed in the reaction of nickelocene with vinyllit
hium or -magnesium compounds. CpNi(vinyl) reacts further to form pi-al
lyl complexes and other compounds not yet fully characterized. For R'
= CH3, pi-allyl complex 1 is formed and for R' = C6H5 two pi-allyl iso
mers anti-2a and syn-2b are formed. The mechanisms of alpha-, beta-, g
amma- and eta-H elimination and of hydrogen transfer reactions are dis
cussed.