Development of an effective and stable catalyst for water oxidation is one of the main challenges in the establishment of a practical solar fuel scheme. The oxidation half-reaction involves two water molecules, rearrangement of multiple bonds, and transfer of four electrons and four protons. A practical catalyst must be highly active, yet stable over prolonged periods under harsh, oxidative conditions. Furthermore, it is highly desirable that the catalyst only incorporates abundant elements to enable large-scale applications. A number of catalytic systems for water oxidation, both heterogeneous and homogeneous, have been described. Heterogeneous metal-oxide catalysts are comparatively stable and synthetically accessible. However, property tuning, characterization, and mechanistic studies are challenging for these inorganic phases. Conversely, molecular catalysts are kinetically faster, and can be tailored using the formidable arsenal of synthetic organic chemistry. This enables rational design of catalysts based on mechanistic hypotheses. Practically, the application of molecular catalysts is limited by their stability under harsh oxidative conditions.<br/>In this presentation, I shall describe water electrooxidation catalyzed by surface-adsorbed complexes of cobalt with a range of perfluorinated ligands. Immobilization is accomplished by drop casting, without linker groups or surface modification. The catalysts are exceptionally active and stable stabile (on par with fully-inorganic catalysts reported previously).

Perfluorinated phthalocyanines and other ligands for efficient co-catalyzed electrooxidation of water

249th National Meeting (2015)

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