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A cyclohexyl based pincer phosphine ligand undergoes cyclometalation with an iridium cyclooctadiene precursor to give a highly thermally stable iridium(III) complex where a C(sp3)–H bond has been oxidatively added. This iridium(III) hydride complex is reduced with potassium to give a terminal iridium(I) dinitrogen complex with no tendency to dimerization. The corresponding cyclohexyl phosphinite ligand undergoes reversible dehydrogenation to give the aromatic cyclometalated iridium(III) hydride complex together with 3 equivalents of dihydrogen.
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