Me 5 )ClIr] + with 2,2′-bipyridine and related aromatic ligands show only the expected Cl/H exchange on reaction with borohydrides, the systems [(RNdCHCHd NR)(η 5 -C 5 Me 5 )ClIr] + undergo reduction to the enediamido(2-)-iridium(III) species [(RNCHdCHNR)(η 5 -C 5 -Me 5 )Ir], even in protic media, if R is an axially shielding 2,6-dialkylphenyl group. In protic media the complex ion with R ) cyclohexyl undergoes Cl/H exchange and stepwise hydrogenation of the R-diimine ligand via [(RHNCH 2 CHdNR)(η 5 -C 5 Me 5 )HIr](PF 6 ) to the structurally characterized compound [(RHNCH 2 CH 2 NHR)(η 5 -C 5 Me 5 )HIr][BH 3 (CN)].
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