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

Abstract

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/cm 2 irradiation are observed for core/shell structures compared to TiO 2 after derivatization with [Ru(4,4$$'$$-PO 3H 2bpy) 2(bpy)] 2+ (RuP 2) 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$$|$$TiO 2|-RuP 2,IrO 2, 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 TiO 2 to stabilize surface binding of -RuP 2 prior to the addition of the IrO X NPs.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1386918
Grant/Contract Number:  
SC0001011
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal 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; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
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; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly)

Citation Formats

Michaux, Katherine E., Gambardella, Alessa A., Alibabaei, Leila, Ashford, Dennis L., Sherman, Benjamin D., Binstead, Robert A., Meyer, Thomas J., and Murray, Royce W. Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst. United States: N. p., 2015. Web. doi:10.1021/acs.jpcc.5b05711.
Michaux, Katherine E., Gambardella, Alessa A., Alibabaei, Leila, Ashford, Dennis L., Sherman, Benjamin D., Binstead, Robert A., Meyer, Thomas J., & Murray, Royce W. Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst. United States. https://doi.org/10.1021/acs.jpcc.5b05711
Michaux, Katherine E., Gambardella, Alessa A., Alibabaei, Leila, Ashford, Dennis L., Sherman, Benjamin D., Binstead, Robert A., Meyer, Thomas J., and Murray, Royce W. Wed . "Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst". United States. https://doi.org/10.1021/acs.jpcc.5b05711. https://www.osti.gov/servlets/purl/1386918.
@article{osti_1386918,
title = {Visible Photoelectrochemical Water Splitting Based on a Ru(II) Polypyridyl Chromophore and Iridium Oxide Nanoparticle Catalyst},
author = {Michaux, Katherine E. and Gambardella, Alessa A. and Alibabaei, Leila and Ashford, Dennis L. and Sherman, Benjamin D. and Binstead, Robert A. and Meyer, Thomas J. and Murray, Royce W.},
abstractNote = {Preparation of Ru(II) polypyridyl-iridium oxide nanoparticle (IrOX 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 IrOX 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 IrOX NPs.},
doi = {10.1021/acs.jpcc.5b05711},
url = {https://www.osti.gov/biblio/1386918}, journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 29,
volume = 119,
place = {United States},
year = {2015},
month = {7}
}

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Cited by: 25 works
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Works referencing / citing this record:

Hybrid photoanodes for water oxidation combining a molecular photosensitizer with a metal oxide oxygen-evolving catalyst
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A stable dye-sensitized photoelectrosynthesis cell mediated by a NiO overlayer for water oxidation
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Titanium dioxide thin films by atomic layer deposition: a review
journal, August 2017