It has been well established that high valent metal-oxo species are important intermediates in a large number of biologically and industrially important chemical transformations. To date, the majority of such compounds possess early transition metal centers, and thus generate electron deficient M-O moieties that react in an electrophilic manner. In contrast, the existence of late first row transitions metal complexes bearing M-O moieties has not been well established. This is consistent with the fact such species should possess much more electron rich M-O moieties, and thus will readily react with electrophilic compounds. In addition, such complexes when formed should have reactivity patterns distinct from those of the early first row transition metal congeners. This is especially true of M-O species possessing tetragonal symmetry, where considerations concerning fundamental bonding properties would preclude their existence (the concept of the oxo-wall). In this work we will provide experimental evidence for the existence of late first-row transition metal complexes that <i>apparently</i> circumvent the oxo-wall, and have reactivity patterns that would be expected of early transition metal species. In addition, we will examine the mechanism of formal H- and O-atom transfer reactions promoted by such species.

Mechanism of exogenous substrate oxidation by oxidized Co and Ni species bearing M-O moieties

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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