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Issue 11, 2015
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Synthesis, characterization, and water oxidation by a molecular chromophore-catalyst assembly prepared by atomic layer deposition. The “mummy” strategy

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Abstract

A new strategy for preparing spatially-controlled, multi-component films consisting of molecular light absorbing chromophores and water oxidation catalysts on high surface area, mesoporous metal oxide surfaces is described. Atomic layer deposition (ALD) is used to embed a surface-bound chromophore in a thin layer of inert Al2O3, followed by catalyst binding to the new oxide surface. In a final step, catalyst surface-binding is stabilized by a subsequent ALD overlayer of Al2O3. The ALD assembly procedure bypasses synthetic difficulties arising from the preparation of phosphonic acid derivatized, covalently-linked assemblies. An ALD mummy-based assembly has been used to demonstrate photoelectrochemical dehydrogenation of hydroquinone. Electrocatalytic water oxidation at pH 8.8 is observed over a 2 hour electrolysis period and light-assisted water oxidation over a 6 hour photolysis period with O2 detected with a generator–collector electrode configuration.

Graphical abstract: Synthesis, characterization, and water oxidation by a molecular chromophore-catalyst assembly prepared by atomic layer deposition. The “mummy” strategy

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Publication details

The article was received on 13 May 2015, accepted on 30 Jul 2015 and first published on 31 Jul 2015


Article type: Edge Article
DOI: 10.1039/C5SC01752A
Citation: Chem. Sci., 2015,6, 6398-6406
  • Open access: Creative Commons BY license
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    Synthesis, characterization, and water oxidation by a molecular chromophore-catalyst assembly prepared by atomic layer deposition. The “mummy” strategy

    A. M. Lapides, B. D. Sherman, M. K. Brennaman, C. J. Dares, K. R. Skinner, J. L. Templeton and T. J. Meyer, Chem. Sci., 2015, 6, 6398
    DOI: 10.1039/C5SC01752A

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