Water oxidation is a mechanistically and energetically demanding reaction, making design of water oxidation catalysts for artificial photosynthesis a significant challenge. However, the natural Mn4CaOx oxygen-evolving complex (OEC) and the Co4O4 clusters found in Co-Pi and other cobalt oxide catalysts suggest a promising opportunity for new materials.  Since these M4O4 �cubanes� have been proposed to promote high water oxidation activity in their respective systems, molecular models of M4O4 are poised to provide insight on H2O splitting mechanisms and to generate new cataysts. Molecular Mn and Co cubanes were synthesized and used to prepare materials by thermolysis, ligand exchange, atomic layer deposition, and molecular linking strategies. The goal of these efforts is a robust, catalytic material containing intact M4O4 units. The resulting materials were characterized electrochemically and by XAS, XPS, Raman, and other spectroscopies.A portion of the figure is reproduced, with permission, from Kanan, M. W.; Nocera, D. G. Science 2008  , 321, 1072�1075.

Materials for water oxidation prepared from Mn- and Co-oxo cubane molecular precursors

248th National Meeting (2014)

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