The synthesis of the metalhydride Cp*(L')IrH+OTf- (L' = 1-(2-cyclohexenyl)-
3-cyclohexylimidazolin-2-ylidene, OTf = OSO2CF3) is achieved by a cyclohexa
ne to cyclohexene transformation at the N-heterocyclic carbene ligand based
on a CH-activation/beta-hydrogen migration process at the Ir(III) center u
nder mild conditions. The synthetic route to Cp*(L')IrH+OTf- and NMR spectr
oscopic and X-ray structural data are presented.