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Carbon Dioxide Activation

One of the major themes of interest in the Donahue Group is carbon dioxide reduction, particularly its reduction to CO. This interest is motivated by the need to provide renewable carbon feedstock chemicals to replace our finite fossil fuels. Carbon monoxide is a highly desirable product molecule from CO2 activation owing to the ease with which it can be transformed to other molecules, such as methanol.

Our work on the carbon dioxide problem involves two very different projects. One project is a study of low-valent small tungsten complexes that oxidatively add CO2 to form corresponding oxo-carbonyl species. We have recently demonstrated a closed reactivity cycle in which CO2 is reduced to CO and the oxygen atom is removed as H2O (Scheme 1). This work was recently accepted for publication in J. Chem. Soc., Dalton Trans. and selected by the journal editors as a “hot”article.

In continuing efforts on this project, we are looking to perform clean, bulk electrolytic reduction of [WCl4(PMePh2)2], or a suitable variant thereof, to W(II), we are exploring other spectator ligand types that can support the oxidative addition of CO2 to W(II), and we are engaged in a temperature-dependent spectrophotometric study of the oxidative addition of CO2 to [WCl2(PMePh2)4] such that we can determine experimental Ea.

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