Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst

Michaux, Katherine E.; Gambardella, Alessa A.; Alibabaei, Leila; Ashford, Dennis L.; Sherman, Benjamin D.; Binstead, Robert A.; Meyer, Thomas J.; Murray, Royce W.

doi:10.1021/acs.jpcc.5b05711

Title: Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst

Journal Article · Wed Jul 08 00:00:00 EDT 2015 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.5b05711· OSTI ID:1386918

Michaux, Katherine E. ^[1]; Gambardella, Alessa A. ^[1]; Alibabaei, Leila ^[1]; Ashford, Dennis L. ^[1]; Sherman, Benjamin D. ^[1]; Binstead, Robert A. ^[1]; Meyer, Thomas J. ^[1]; Murray, Royce W. ^[1]

Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry

Preparation of Ru(II) polypyridyl-iridium oxide nanoparticle (IrO_X NP) chromophore-catalyst assemblies on an FTO$|nano$ITO$$|$$TiO2 core/shell by a layer-bylayer procedure is described for application in dye-sensitized photoelectrosynthesis cells (DSPEC). Significantly enhanced, bias-dependent photocurrents with Lumencor 455 nm 14.5 mW/cm² irradiation are observed for core/shell structures compared to TiO² after derivatization with [Ru(4,4$$'$$-PO₃H₂bpy)₂(bpy)]²⁺ (RuP₂) and uncapped IrO_X NPs at pH 5.8 in NaSiF6 buffer with a Pt cathode. Photocurrents arising from photolysis of the resulting photoanodes, FTO$|nano$ITO$$|$$TiO₂|-RuP₂,IrO₂, are dependent on TiO2 shell thickness and applied bias, reaching 0.2 mA/cm2 at 0.5 V vs AgCl/Ag with a shell thickness of 6.6 nm. Long-term photolysis in the NaSiF6 buffer results in a marked decrease in photocurrent over time due to surface hydrolysis and loss of the chromophore from the surface. Long-term stability, with sustained photocurrents, has been obtained by atomic layer deposition (ALD) of overlayers of TiO₂ to stabilize surface binding of -RuP₂ prior to the addition of the IrO_X NPs.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001011

OSTI ID:: 1386918

Journal Information:: Journal of Physical Chemistry. C, Vol. 119, Issue 29; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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A stable dye-sensitized photoelectrosynthesis cell mediated by a NiO overlayer for water oxidation Wang, Degao; Niu, Fujun; Mortelliti, Michael J. Proceedings of the National Academy of Sciences, Vol. 117, Issue 23 https://doi.org/10.1073/pnas.1821687116	journal	September 2019
Hybrid photoanodes for water oxidation combining a molecular photosensitizer with a metal oxide oxygen-evolving catalyst Collomb, Marie-Noëlle; Morales, Daniela V.; Astudillo, Catalina N. Sustainable Energy & Fuels, Vol. 4, Issue 1 https://doi.org/10.1039/c9se00597h	journal	January 2020
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (homogeneous)
catalysis (heterogeneous)
solar (photovoltaic)
solar (fuels)
photosynthesis (natural and artificial)
hydrogen and fuel cells
electrodes - solar
charge transport
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Title: Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst

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