A new PNP-pincer ligand 1 bearing neopentyl substituents reacted with [Ir(cod)2]BF4 to form hydridoiridacycle 3 via oxidative addition of a C–H bond of a neopentyl group to IrI. Addition of π-acceptor ligands induced C–H reductive elimination to form cationic iridium(I) complexes 5 ligated by the π-acceptor ligand. Although 3 did not give a benzene adduct, reaction of 3 with nitrobenzene or acetophenone afforded the C–H activated 7a or 8a.
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