Abstract
The iridium(iii/iv/v) imido redox series Ir(NtBu)N(CHCHPtBu2)20/+/2+ was synthesized and examined spectroscopically, magnetically, crystallographically and computationally. The monocationic iridium(iv) imide exhibits an electronic doublet ground state with considerable 'imidyl' character as a result of covalent Ir-NtBu bonding. Reduction gives the neutral imide Ir(NtBu)N(CHCHPtBu2)2 as the first example of an iridium complex with a triplet ground state. Its reactivity with respect to nitrene transfer to selected electrophiles (CO2) and nucleophiles (PMe3), respectively, is reported.
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