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A Molecular Silane-Derivatized Ru(II) Catalyst for Photoelectrochemical Water Oxidation

  • Lei Wu
    Lei Wu
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
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  • , 
  • Michael Eberhart
    Michael Eberhart
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
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  • , 
  • Animesh Nayak
    Animesh Nayak
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
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  • , 
  • M. Kyle Brennaman
    M. Kyle Brennaman
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
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  • , 
  • Bing Shan
    Bing Shan
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
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  • , and 
  • Thomas J. Meyer*
    Thomas J. Meyer
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
    *[email protected]
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    Orcidhttp://orcid.org/0000-0002-7006-2608
Cite this: J. Am. Chem. Soc. 2018, 140, 44, 15062–15069
Publication Date (Web):October 16, 2018
https://doi.org/10.1021/jacs.8b10132
Copyright © 2018 American Chemical Society
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    Abstract

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    Photoanodes in dye-sensitized photoelectrosynthesis cells integrate molecular chromophore/catalyst assemblies on mesoporous n-type metal oxide electrodes for light-driven water oxidation. One limitation for sustainable photoanodes is the stability of chromophore/catalyst assembly on electrode surfaces for long periods. Progress has been made in stabilizing chromophores based on atomic layer deposition, polymer dip coating, C–C cross-coupling by electropolymerization, and silane surface binding, but little progress has been made on catalyst stabilization. We report here the silane-derivatized catalyst, Ru(bda)(L)2 (bda = 2,2′-bipyridine-6,6′-dicarboxylate, L = 4-(6-(triethoxysilyl)hexyl)pyridine), catalyst 1, which is stabilized on metal oxide electrode surfaces over an extended pH range. A surface stabilization study shows that it maintains its reactivity on the electrode surface toward electrochemical oxidation over a wide range of conditions. Its electrochemical stability on electrode surfaces has been systematically evaluated, and its role as a catalyst for water oxidation has been explored. On surfaces of mesoporous nanostructured core/shell SnO2/TiO2, with a TiO2 stabilized inner layer of the Ru(II) polypyridyl chromophore, [Ru(4,4′-(PO3H2)2bpy)(bpy)2]2+ (RuP2+; bpy = 2,2′-bipyridine), highly efficient photoelectrochemical water oxidation catalysis occurs to produce O2 with a maximum efficiency of ∼1.25 mA/cm2. Long-term loss of catalytic activity occurs with time owing to catalyst loss from the electrode surface by axial ligand dissociation in the high oxidation states of the catalyst.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b10132.

    • NMR spectra of 4-(hex-5-en-1-yl)pyridine and 4-(6-(triethoxysilyl)hexyl)pyridine, ESI-MS and NMR analysis of the catalyst 1 (PDF)

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