The transition-metal catalyzed activation of hydrogen and reduction of protons proceeds via metal-hydride intermediates. The formation—and reactivity—of these metal hydride complexes involves proton-coupled electron transfer (PCET) processes that can proceed through stepwise or concerted routes. Using a combination of electrochemical and time-resolved spectroscopic techniques, we investigated the details of the PCET reactivity involved in the activation of a transition metal hydride complex (CpW(CO)<sub>2</sub>(PMe<sub>3</sub>)H). We find that both the reaction mechanism and kinetics of elementary steps are influenced by the strength of the base and the oxidant employed, demonstrating that reactivity can be tuned and controlled across a two-dimensional parameter space.

Proton-coupled electron transfer activation of a tungsten hydride complex

256th National Meeting (2018)

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