Fundamental processes such as photoinduced electron transfer, charge separation, and efficient dioxygen and dihydrogen production need to be understood in order to design effective water splitting catalysts. We are merging synthetic, redox-, spectroscopic-, surface-, and computater-based techniques with the aim to incorporate reactive sites, antennae, and acceptors in multimetallic complexes. Current efforts will be discussed in this talk, focusing on dioxygen generation based on ruthenium systems, as well as on dihydrogen generation based on cobalt and ruthenium/cobalt systems.  For dioxygen generation we will discuss (i) the development of new ruthenium catalytic modules that enable physisorption on redox substrates as LB films, and (ii) the requirements for formation of six-coordinate manganese(IV) in electroactive [N2O3] donor type ligands. For dihydrogen generation, we will discuss (i) mechanistic studies on cobalt/oxime species and (iv) progress toward the synthesis and electronic characterization of ruthenium/cobalt systems. Funding DOE

New modules for multimetallic water splitting: Electronic, amphiphilic, and catalytic properties

246th National Meeting (2013)

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