Stepwise hydrogenation of an arylthiophosphinidene isocyanide complex to give tethered aldimine and aminocarbene functions.

The sequential addition of H⁺ and H⁻ ions to [Mo₂Cp₂(μ-κ²P,S:κ¹P,η⁴-SPMes*)(CNtBu)(CO)₂] (Mes* = 2,4,6-C₆H₂tBu₃) completes a hydrocarbation or hydronitration of the uncoordinated C=C bond of the Mes* ring, yielding new ligands with thiophosphinidene and aldimine or aminocarbene functions tethered to a η⁴-cyclohexadiene ring. The H⁻ ion first attacks a Cp group to give a cyclopentadiene complex which evolves via a hydride intermediate.