Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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 (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.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  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:
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.
Copy to clipboard
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
Copy to clipboard
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.
Copy to clipboard
@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},
journal = {Journal of Physical Chemistry. C},
number = 29,
volume = 119,
place = {United States},
year = {Wed Jul 08 00:00:00 EDT 2015},
month = {Wed Jul 08 00:00:00 EDT 2015}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpcc.5b05711
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 31 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Solar water splitting in a molecular photoelectrochemical cell
journal, November 2013

  • Alibabaei, L.; Brennaman, M. K.; Norris, M. R.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 50
  • DOI: 10.1073/pnas.1319628110

Chemical Approaches to Artificial Photosynthesis. 2
journal, October 2005

  • Alstrum-Acevedo, James H.; Brennaman, M. Kyle; Meyer, Thomas J.
  • Inorganic Chemistry, Vol. 44, Issue 20
  • DOI: 10.1021/ic050904r

Oxidizing water two ways
journal, September 2011

Photoassisted Overall Water Splitting in a Visible Light-Absorbing Dye-Sensitized Photoelectrochemical Cell
journal, January 2009

  • Youngblood, W. Justin; Lee, Seung-Hyun Anna; Kobayashi, Yoji
  • Journal of the American Chemical Society, Vol. 131, Issue 3, p. 926-927
  • DOI: 10.1021/ja809108y

Metal oxides as heterogeneous catalysts for oxygen evolution under photochemical conditions
journal, January 1988

  • Harriman, Anthony; Pickering, Ingrid J.; Thomas, John M.
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 84, Issue 8
  • DOI: 10.1039/f19888402795

Bidentate Dicarboxylate Capping Groups and Photosensitizers Control the Size of IrO 2 Nanoparticle Catalysts for Water Oxidation †
journal, June 2007

  • Hoertz, Paul G.; Kim, Yeong-Il; Youngblood, W. Justin
  • The Journal of Physical Chemistry B, Vol. 111, Issue 24
  • DOI: 10.1021/jp070735r

Kinetics of Electron Transfer and Oxygen Evolution in the Reaction of [Ru(bpy) 3 ] 3+ with Colloidal Iridium Oxide
journal, October 2004

  • Morris, Natalie D.; Suzuki, Masahiro; Mallouk, Thomas E.
  • The Journal of Physical Chemistry A, Vol. 108, Issue 42
  • DOI: 10.1021/jp0480145

Efficient Electro-Oxidation of Water near Its Reversible Potential by a Mesoporous IrO x Nanoparticle Film
journal, July 2009

  • Nakagawa, Takaaki; Beasley, Christopher A.; Murray, Royce W.
  • The Journal of Physical Chemistry C, Vol. 113, Issue 30
  • DOI: 10.1021/jp9060076

A High Yield Synthesis of Ligand-Free Iridium Oxide Nanoparticles with High Electrocatalytic Activity
journal, February 2011

  • Zhao, Yixin; Hernandez-Pagan, Emil A.; Vargas-Barbosa, Nella M.
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 5
  • DOI: 10.1021/jz200051c

Anodic Deposition of Colloidal Iridium Oxide Thin Films from Hexahydroxyiridate(IV) Solutions
journal, June 2011

  • Zhao, Yixin; Vargas-Barbosa, Nella M.; Hernandez-Pagan, Emil A.
  • Small, Vol. 7, Issue 14
  • DOI: 10.1002/smll.201100485

Characterization of an Amorphous Iridium Water-Oxidation Catalyst Electrodeposited from Organometallic Precursors
journal, January 2013

  • Blakemore, James D.; Mara, Michael W.; Kushner-Lenhoff, Maxwell N.
  • Inorganic Chemistry, Vol. 52, Issue 4
  • DOI: 10.1021/ic301968j

Comparison of Amorphous Iridium Water-Oxidation Electrocatalysts Prepared from Soluble Precursors
journal, April 2012

  • Blakemore, James D.; Schley, Nathan D.; Kushner-Lenhoff, Maxwell N.
  • Inorganic Chemistry, Vol. 51, Issue 14
  • DOI: 10.1021/ic300764f

Photovoltage Effects of Sintered IrO 2 Nanoparticle Catalysts in Water-Splitting Dye-Sensitized Photoelectrochemical Cells
journal, April 2014

  • Swierk, John R.; McCool, Nicholas S.; Saunders, Timothy P.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 30
  • DOI: 10.1021/jp500589n

Formation of Iridium(IV) Oxide (IrO X ) Films by Electroflocculation
journal, September 2013

  • Michaux, Katherine E.; Murray, Royce W.
  • Langmuir, Vol. 29, Issue 39
  • DOI: 10.1021/la4025876

Atomic Layer Deposition of TiO 2 on Mesoporous nanoITO: Conductive Core–Shell Photoanodes for Dye-Sensitized Solar Cells
journal, May 2014

  • Alibabaei, Leila; Farnum, Byron H.; Kalanyan, Berç
  • Nano Letters, Vol. 14, Issue 6
  • DOI: 10.1021/nl5006433

Stabilization of [Ru(bpy) 2 (4,4′-(PO 3 H 2 )bpy)] 2+ on Mesoporous TiO 2 with Atomic Layer Deposition of Al 2 O 3
journal, December 2012

  • Hanson, Kenneth; Losego, Mark D.; Kalanyan, Berç
  • Chemistry of Materials, Vol. 25, Issue 1
  • DOI: 10.1021/cm303172w

Stabilizing Small Molecules on Metal Oxide Surfaces Using Atomic Layer Deposition
journal, September 2013

  • Hanson, Kenneth; Losego, Mark D.; Kalanyan, Berç
  • Nano Letters, Vol. 13, Issue 10
  • DOI: 10.1021/nl402416s

Crossing the divide between homogeneous and heterogeneous catalysis in water oxidation
journal, November 2013

  • Vannucci, A. K.; Alibabaei, L.; Losego, M. D.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 52
  • DOI: 10.1073/pnas.1319832110

Effective Panchromatic Sensitization of Electrochemical Solar Cells: Strategy and Organizational Rules for Spatial Separation of Complementary Light Harvesters on High-Area Photoelectrodes
journal, November 2012

  • Jeong, Nak Cheon; Son, Ho-Jin; Prasittichai, Chaiya
  • Journal of the American Chemical Society, Vol. 134, Issue 48
  • DOI: 10.1021/ja308725r

Radial Electron Collection in Dye-Sensitized Solar Cells
journal, September 2008

  • Martinson, Alex B. F.; Elam, Jeffrey W.; Liu, Jun
  • Nano Letters, Vol. 8, Issue 9, p. 2862-2866
  • DOI: 10.1021/nl8015285

Glass-Encapsulated Light Harvesters: More Efficient Dye-Sensitized Solar Cells by Deposition of Self-Aligned, Conformal, and Self-Limited Silica Layers
journal, May 2012

  • Son, Ho-Jin; Wang, Xinwei; Prasittichai, Chaiya
  • Journal of the American Chemical Society, Vol. 134, Issue 23
  • DOI: 10.1021/ja300015n

Fast Transporting ZnO–TiO 2 Coaxial Photoanodes for Dye-Sensitized Solar Cells Based on ALD-Modified SiO 2 Aerogel Frameworks
journal, June 2012

  • Williams, Vennesa O.; Jeong, Nak Cheon; Prasittichai, Chaiya
  • ACS Nano, Vol. 6, Issue 7
  • DOI: 10.1021/nn3015695

Dye Stabilization and Enhanced Photoelectrode Wettability in Water-Based Dye-Sensitized Solar Cells through Post-assembly Atomic Layer Deposition of TiO 2
journal, July 2013

  • Son, Ho-Jin; Prasittichai, Chaiya; Mondloch, Joseph E.
  • Journal of the American Chemical Society, Vol. 135, Issue 31
  • DOI: 10.1021/ja406538a

Synthesis of Phosphonic Acid Derivatized Bipyridine Ligands and Their Ruthenium Complexes
journal, October 2013

  • Norris, Michael R.; Concepcion, Javier J.; Glasson, Christopher R. K.
  • Inorganic Chemistry, Vol. 52, Issue 21
  • DOI: 10.1021/ic4014976

Die Oxyde des Iridiums
journal, March 1908

Stabilizing chromophore binding on TiO 2 for long-term stability of dye-sensitized solar cells using multicomponent atomic layer deposition
journal, January 2014

  • Kim, Do Han; Losego, Mark D.; Hanson, Kenneth
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 18
  • DOI: 10.1039/C4CP01130A
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    A stable dye-sensitized photoelectrosynthesis cell mediated by a NiO overlayer for water oxidation
    journal, September 2019

    • Wang, Degao; Niu, Fujun; Mortelliti, Michael J.
    • Proceedings of the National Academy of Sciences, Vol. 117, Issue 23
    • DOI: 10.1073/pnas.1821687116

    Hybrid photoanodes for water oxidation combining a molecular photosensitizer with a metal oxide oxygen-evolving catalyst
    journal, January 2020

    • Collomb, Marie-Noëlle; Morales, Daniela V.; Astudillo, Catalina N.
    • Sustainable Energy & Fuels, Vol. 4, Issue 1
    • DOI: 10.1039/c9se00597h

    Titanium dioxide thin films by atomic layer deposition: a review
    journal, August 2017

    • Niemelä, Janne-Petteri; Marin, Giovanni; Karppinen, Maarit
    • Semiconductor Science and Technology, Vol. 32, Issue 9
    • DOI: 10.1088/1361-6641/aa78ce
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: