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A [16 + 1] valence electron configured rhodium aminyl radical complex could be synthesized and characterized in detail by pulse EPR spectroscopy and DFT calculations. The unpaired electron is delocalized over the metal center and two adjacent nitrogens. H-abstraction reactions from thiols and triethylsilane show that the spin density is predominantly localized on both nitrogens.

A little goes a long way: An iridium–nitrogen‐radical complex is a highly active and selective catalyst for the dehydrogenation (oxidation) of primary alcohols to aldehydes in the presence of the oxidant benzoquinone (see simplified scheme). With only 0.01 mol % of the complex, turnover frequencies of up to 150 000 s−1 are reached.

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