Late metal oxo and nitrido complexes are attractive intermediates for the oxidation of organic compounds, but they are typically inaccessible due to the incompatibility of strong metal-ligand π bonding with the high d electron counts found in late metal complexes (the “oxo wall”). Here we describe attempts to use iminoxolene ligands (iminoxolene = o-C6R4(O)(NAr)) to support square pyramidal iridium complexes that contain reactive oxo or nitrido groups. Computational data support the surprising notion that the role of the iminoxolenes is to accept electron density from the metal to allow access to these high-valent intermediates. Data supporting the identification of reactive intermediates as terminal oxo or nitrido complexes, as well as mechanistic data about their oxidative reactivity, will be presented.

Using iminoxolene supporting ligands to access high-valent iridium oxo and nitrido complexes for oxidation of organics

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