New Approaches to Reversible Homogeneous Electrocatalysts

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In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Robert Waymouth of Stanford University is developing new experimental approaches for the electrocatalytic conversion of alcohols into ketones. The conversion of chemical compounds such as alcohols into ketones can form the basis of fuel cells, which are alternatives to conventional power sources. While the alcohol/ketone fuel cells are very attractive, the chemical reaction is difficult. In this project, new catalysts that facilitate such difficult reactions are being developed. This research provides new means for the energy-efficient conversion of chemical fuels into useful forms of energy. Collaborative investigations with Professors Richard Zare and Christopher Chidsey at Stanford University enhance the experimental and educational infrastructure for energy science and provide faculty, postdoctoral, graduate, and undergraduate students with rich opportunities for education and collaborative research. This project focuses on homogeneous catalysts bearing proton and redox-active ligands. It is guided by the hypothesis that mechanistic concepts that have been developed for chemical transfer hydrogenation catalysis, such as metal-ligand bifunctional activation of substrates, can be applied to the behavior of proton- and redox-active ligands that are effective in mediating multi-electron and proton transfers. The experimental approach utilizes homogeneous coordination complexes and seeks to determine the key features of the metal/ligand coordination environments that mediate the hydrogen atom, proton and electron transfer steps in efficient electrocatalytic processes. The development and application of high resolution mass spectrometry techniques, interfaced to electrochemical cells is an innovative aspect of the experimental plan. These provide new mechanistic insights on the intermediates generated during electrocatalytic reactions. Broader impacts of this work include new approaches for the energy-efficient conversion of chemical fuels into useful forms of energy.