Metal peroxides are key intermediates implicated in the mechanisms of oxygenase enzymes, and are important species in energy storage technologies. Rare-earth metal (REM) peroxides have been synthesized on RE solid supports through reactions with aqueous hydrogen peroxide at elevated temperatures, and have been shown to oxidize both organic and inorganic substrates, such as carbon monoxide and styrene. However, the properties and reactivity of soluble trivalent REM peroxides have received much less attention, since their syntheses often resulted from accidental exposure of divalent REMs to dioxygen (O2). This is due to the absence of reproducible, high-yielding synthetic procedures to form these REM peroxides from redox-inactive trivalent REM precursors, which is additionally complicated by their energetic preference to form insoluble aggregates. We recently presented kinetic and mechanistic details of an O2 reduction reaction with trivalent REM triflates that form soluble REM peroxides with &gt;95% selectivity. In this presentation, we will expand upon our previous findings with electrochemical and spectroscopic structural characterization of the REM peroxide products, as well as comment on peroxide reactivity with Brønsted acid and organic substrates.

Synthesis, characterization and reactivity of soluble rare-earth peroxides via Lewis-acid promoted oxygen reduction

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

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.