Visible photoelectrochemical water splitting into H 2 and O 2 in a dye-sensitized photoelectrosynthesis cell
Abstract
A hybrid strategy for solar water splitting is exploited here based on a dye-sensitized photoelectrosynthesis cell (DSPEC) with a mesoporous SnO 2/TiO 2 core/shell nanostructured electrode derivatized with a surface-bound Ru(II) polypyridyl-based chromophore–catalyst assembly. The assembly, [(4,4’-(PO 3H 2) 2bpy) 2Ru(4-Mebpy-4’-bimpy)Ru(tpy)(OH 2)] 4+ ([RuaII-RubII-OH 2] 4+, combines both a light absorber and a water oxidation catalyst in a single molecule. It was attached to the TiO 2 shell by phosphonate-surface oxide binding. The oxide-bound assembly was further stabilized on the surface by atomic layer deposition (ALD) of either Al 2O 3 or TiO 2 overlayers. Illumination of the resulting fluorine-doped tin oxide (FTO)|SnO 2/TiO 2|-[Ru a II-Ru b II-OH 2] 4+(Al 2O 3 or TiO 2) photoanodes in photoelectrochemical cells with a Pt cathode and a small applied bias resulted in visible-light water splitting as shown by direct measurements of both evolved H 2 and O 2. The performance of the resulting DSPECs varies with shell thickness and the nature and extent of the oxide overlayer. Use of the SnO 2/TiO 2 core/shell compared with nanoITO/TiO 2 with the same assembly results in photocurrent enhancements of ~5. In conclusion, systematic variations in shell thickness and ALD overlayer lead to photocurrentmore »
- Authors:
-
- Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
- Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC). Center for Solar Fuels (UNC EFRC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Contributing Org.:
- 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
- OSTI Identifier:
- 1210802
- Grant/Contract Number:
- SC0001011
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Volume: 112; Journal Issue: 19; Journal ID: ISSN 0027-8424
- Publisher:
- National Academy of Sciences, Washington, DC (United States)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 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
Alibabaei, Leila, Sherman, Benjamin D., Norris, Michael R., Brennaman, M. Kyle, and Meyer, Thomas J. Visible photoelectrochemical water splitting into H2 and O2 in a dye-sensitized photoelectrosynthesis cell. United States: N. p., 2015.
Web. doi:10.1073/pnas.1506111112.
Alibabaei, Leila, Sherman, Benjamin D., Norris, Michael R., Brennaman, M. Kyle, & Meyer, Thomas J. Visible photoelectrochemical water splitting into H2 and O2 in a dye-sensitized photoelectrosynthesis cell. United States. https://doi.org/10.1073/pnas.1506111112
Alibabaei, Leila, Sherman, Benjamin D., Norris, Michael R., Brennaman, M. Kyle, and Meyer, Thomas J. Mon .
"Visible photoelectrochemical water splitting into H2 and O2 in a dye-sensitized photoelectrosynthesis cell". United States. https://doi.org/10.1073/pnas.1506111112. https://www.osti.gov/servlets/purl/1210802.
@article{osti_1210802,
title = {Visible photoelectrochemical water splitting into H2 and O2 in a dye-sensitized photoelectrosynthesis cell},
author = {Alibabaei, Leila and Sherman, Benjamin D. and Norris, Michael R. and Brennaman, M. Kyle and Meyer, Thomas J.},
abstractNote = {A hybrid strategy for solar water splitting is exploited here based on a dye-sensitized photoelectrosynthesis cell (DSPEC) with a mesoporous SnO2/TiO2 core/shell nanostructured electrode derivatized with a surface-bound Ru(II) polypyridyl-based chromophore–catalyst assembly. The assembly, [(4,4’-(PO3H2)2bpy)2Ru(4-Mebpy-4’-bimpy)Ru(tpy)(OH2)]4+ ([RuaII-RubII-OH2]4+, combines both a light absorber and a water oxidation catalyst in a single molecule. It was attached to the TiO2 shell by phosphonate-surface oxide binding. The oxide-bound assembly was further stabilized on the surface by atomic layer deposition (ALD) of either Al2O3 or TiO2 overlayers. Illumination of the resulting fluorine-doped tin oxide (FTO)|SnO2/TiO2|-[RuaII-RubII-OH2]4+(Al2O3 or TiO2) photoanodes in photoelectrochemical cells with a Pt cathode and a small applied bias resulted in visible-light water splitting as shown by direct measurements of both evolved H2 and O2. The performance of the resulting DSPECs varies with shell thickness and the nature and extent of the oxide overlayer. Use of the SnO2/TiO2 core/shell compared with nanoITO/TiO2 with the same assembly results in photocurrent enhancements of ~5. In conclusion, systematic variations in shell thickness and ALD overlayer lead to photocurrent densities as high as 1.97 mA/cm2 with 445-nm, ~90-mW/cm2 illumination in a phosphate buffer at pH 7.},
doi = {10.1073/pnas.1506111112},
url = {https://www.osti.gov/biblio/1210802},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 19,
volume = 112,
place = {United States},
year = {2015},
month = {4}
}
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Works referenced in this record:
Chemical approaches to artificial photosynthesis
journal, September 2012
- Concepcion, J. J.; House, R. L.; Papanikolas, J. M.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 39
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
Solar Water Splitting Cells
journal, November 2010
- Walter, Michael G.; Warren, Emily L.; McKone, James R.
- Chemical Reviews, Vol. 110, Issue 11, p. 6446-6473
Powering the planet: Chemical challenges in solar energy utilization
journal, October 2006
- Lewis, N. S.; Nocera, D. G.
- Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735
Energy and environment policy case for a global project on artificial photosynthesis
journal, January 2013
- Faunce, Thomas A.; Lubitz, Wolfgang; Rutherford, A. W. (Bill)
- Energy & Environmental Science, Vol. 6, Issue 3
Applications of metal oxide materials in dye sensitized photoelectrosynthesis cells for making solar fuels: let the molecules do the work
journal, January 2013
- Alibabaei, Leila; Luo, Hanlin; House, Ralph L.
- Journal of Materials Chemistry A, Vol. 1, Issue 13
Visible Region Photooxidation on TiO 2 with a Chromophore−Catalyst Molecular Assembly
journal, October 1999
- Treadway, Joseph A.; Moss, John A.; Meyer, Thomas J.
- Inorganic Chemistry, Vol. 38, Issue 20
Making solar fuels by artificial photosynthesis
journal, March 2011
- Song, Wenjing; Chen, Zuofeng; Brennaman, M. Kyle
- Pure and Applied Chemistry, Vol. 83, Issue 4
Visible Light-Driven Water Splitting in Photoelectrochemical Cells with Supramolecular Catalysts on Photoanodes
journal, May 2014
- Ding, Xin; Gao, Yan; Zhang, Linlin
- ACS Catalysis, Vol. 4, Issue 7
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
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
Effect of an Ultrathin TiO2 Layer Coated on Submicrometer-Sized ZnO Nanocrystallite Aggregates by Atomic Layer Deposition on the Performance of Dye-Sensitized Solar Cells
journal, April 2010
- Park, Kwangsuk; Zhang, Qifeng; Garcia, Betzaida Battalla
- Advanced Materials, Vol. 22, Issue 21, p. 2329-2332
Visible Light Driven Benzyl Alcohol Dehydrogenation in a Dye-Sensitized Photoelectrosynthesis Cell
journal, June 2014
- Song, Wenjing; Vannucci, Aaron K.; Farnum, Byron H.
- Journal of the American Chemical Society, Vol. 136, Issue 27
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
Low-Temperature Crystalline Titanium Dioxide by Atomic Layer Deposition for Dye-Sensitized Solar Cells
journal, January 2013
- Chandiran, Aravind Kumar; Yella, Aswani; Stefik, Morgan
- ACS Applied Materials & Interfaces, Vol. 5, Issue 8
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
A visible light water-splitting cell with a photoanode formed by codeposition of a high-potential porphyrin and an iridium water-oxidation catalyst
journal, January 2011
- Moore, Gary F.; Blakemore, James D.; Milot, Rebecca L.
- Energy & Environmental Science, Vol. 4, Issue 7
Polyoxometalate water oxidation catalysts and the production of green fuel
journal, January 2012
- Lv, Hongjin; Geletii, Yurii V.; Zhao, Chongchao
- Chemical Society Reviews, Vol. 41, Issue 22, p. 7572-7589
Visible Light Driven Water Splitting in a Molecular Device with Unprecedentedly High Photocurrent Density
journal, March 2013
- Gao, Yan; Ding, Xin; Liu, Jianhui
- Journal of the American Chemical Society, Vol. 135, Issue 11
Solar Driven Water Oxidation by a Bioinspired Manganese Molecular Catalyst
journal, March 2010
- Brimblecombe, Robin; Koo, Annette; Dismukes, G. Charles
- Journal of the American Chemical Society, Vol. 132, Issue 9
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
Concerted O atom-proton transfer in the O--O bond forming step in water oxidation
journal, April 2010
- Chen, Z.; Concepcion, J. J.; Hu, X.
- Proceedings of the National Academy of Sciences, Vol. 107, Issue 16, p. 7225-7229
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
One-Electron Activation of Water Oxidation Catalysis
journal, May 2014
- Tamaki, Yusuke; Vannucci, Aaron K.; Dares, Christopher J.
- Journal of the American Chemical Society, Vol. 136, Issue 19
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
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
Low-Overpotential Water Oxidation by a Surface-Bound Ruthenium-Chromophore-Ruthenium-Catalyst Assembly
journal, November 2013
- Norris, Michael R.; Concepcion, Javier J.; Fang, Zhen
- Angewandte Chemie International Edition, Vol. 52, Issue 51
Effects of Electron Trapping and Protonation on the Efficiency of Water-Splitting Dye-Sensitized Solar Cells
journal, July 2014
- Swierk, John R.; McCool, Nicholas S.; Saunders, Timothy P.
- Journal of the American Chemical Society, Vol. 136, Issue 31
Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator
journal, April 2012
- Zhao, Y.; Swierk, J. R.; Megiatto, J. D.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 39
Electrochemical Instability of Phosphonate-Derivatized, Ruthenium(III) Polypyridyl Complexes on Metal Oxide Surfaces
journal, May 2015
- Hyde, Jacob T.; Hanson, Kenneth; Vannucci, Aaron K.
- ACS Applied Materials & Interfaces, Vol. 7, Issue 18
Works referencing / citing this record:
A Million Turnover Molecular Anode for Catalytic Water Oxidation
journal, November 2016
- Creus, Jordi; Matheu, Roc; Peñafiel, Itziar
- Angewandte Chemie International Edition, Vol. 55, Issue 49
Ru-bis(pyridine)pyrazolate (bpp)-Based Water-Oxidation Catalysts Anchored on TiO 2 : The Importance of the Nature and Position of the Anchoring Group
journal, February 2016
- Francàs, Laia; Richmond, Craig; Garrido-Barros, Pablo
- Chemistry - A European Journal, Vol. 22, Issue 15
Behavior of Ru-bda Water-Oxidation Catalysts in Low Oxidation States
journal, August 2018
- Matheu, Roc; Ghaderian, Abolfazl; Francàs, Laia
- Chemistry - A European Journal, Vol. 24, Issue 49
Spectroscopic signatures of ligand field states in {Ru II (imine)} complexes
journal, January 2016
- Cadranel, Alejandro; Pieslinger, German E.; Tongying, Pornthip
- Dalton Transactions, Vol. 45, Issue 13
Charge injection into nanostructured TiO 2 electrodes from the photogenerated reduced form of a new Ru( ii ) polypyridine compound: the “anti-biomimetic” mechanism at work
journal, January 2016
- Ronconi, Federico; Santoni, Marie-Pierre; Nastasi, Francesco
- Dalton Transactions, Vol. 45, Issue 36
A Million Turnover Molecular Anode for Catalytic Water Oxidation
journal, November 2016
- Creus, Jordi; Matheu, Roc; Peñafiel, Itziar
- Angewandte Chemie, Vol. 128, Issue 49
Ru-bis(pyridine)pyrazolate (bpp)-Based Water-Oxidation Catalysts Anchored on TiO 2 : The Importance of the Nature and Position of the Anchoring Group
journal, February 2016
- Francàs, Laia; Richmond, Craig; Garrido-Barros, Pablo
- Chemistry - A European Journal, Vol. 22, Issue 15
Behavior of Ru-bda Water-Oxidation Catalysts in Low Oxidation States
journal, August 2018
- Matheu, Roc; Ghaderian, Abolfazl; Francàs, Laia
- Chemistry - A European Journal, Vol. 24, Issue 49
Spectroscopic signatures of ligand field states in {Ru II (imine)} complexes
journal, January 2016
- Cadranel, Alejandro; Pieslinger, German E.; Tongying, Pornthip
- Dalton Transactions, Vol. 45, Issue 13
Charge injection into nanostructured TiO 2 electrodes from the photogenerated reduced form of a new Ru( ii ) polypyridine compound: the “anti-biomimetic” mechanism at work
journal, January 2016
- Ronconi, Federico; Santoni, Marie-Pierre; Nastasi, Francesco
- Dalton Transactions, Vol. 45, Issue 36
A Million Turnover Molecular Anode for Catalytic Water Oxidation
journal, November 2016
- Creus, Jordi; Matheu, Roc; Peñafiel, Itziar
- Angewandte Chemie International Edition, Vol. 55, Issue 49
Solution‐Processed Self‐Powered Transparent Ultraviolet Photodetectors with Ultrafast Response Speed for High‐Performance Communication System
journal, February 2019
- Fang, Huajing; Zheng, Cheng; Wu, Liangliang
- Advanced Functional Materials, Vol. 29, Issue 20
Recent Advances in Sensitized Photocathodes: From Molecular Dyes to Semiconducting Quantum Dots
journal, January 2018
- Wu, Hao-Lin; Li, Xu-Bing; Tung, Chen-Ho
- Advanced Science, Vol. 5, Issue 4
Photoelectrocatalytic Materials for Solar Water Splitting
journal, May 2018
- Yao, Tingting; An, Xiurui; Han, Hongxian
- Advanced Energy Materials, Vol. 8, Issue 21
Light-Driven Water Splitting Mediated by Photogenerated Bromine
journal, March 2018
- Sheridan, Matthew V.; Wang, Ying; Wang, Degao
- Angewandte Chemie International Edition, Vol. 57, Issue 13
Directly Photoexcited Oxides for Photoelectrochemical Water Splitting
journal, September 2019
- Pan, Linfeng; Vlachopoulos, Nick; Hagfeldt, Anders
- ChemSusChem, Vol. 12, Issue 19
Developing a scalable artificial photosynthesis technology through nanomaterials by design
journal, December 2016
- Lewis, Nathan S.
- Nature Nanotechnology, Vol. 11, Issue 12
An aqueous, organic dye derivatized SnO 2 /TiO 2 core/shell photoanode
journal, January 2016
- Wee, Kyung-Ryang; Sherman, Benjamin D.; Brennaman, M. Kyle
- Journal of Materials Chemistry A, Vol. 4, Issue 8
Long-lived charge separation in dye–semiconductor assemblies: a pathway to multi-electron transfer reactions
journal, January 2018
- Sundin, Elin; Abrahamsson, Maria
- Chemical Communications, Vol. 54, Issue 42
Core–shell structured titanium dioxide nanomaterials for solar energy utilization
journal, January 2018
- Li, Wei; Elzatahry, Ahmed; Aldhayan, Dhaifallah
- Chemical Society Reviews, Vol. 47, Issue 22
Dinuclear metal complexes: multifunctional properties and applications
journal, January 2020
- Li, Guangfu; Zhu, Dongxia; Wang, Xinlong
- Chemical Society Reviews, Vol. 49, Issue 3
Ultrathin oxide layers for nanoscale integration of molecular light absorbers, catalysts, and complete artificial photosystems
journal, January 2019
- Katsoukis, Georgios; Frei, Heinz
- The Journal of Chemical Physics, Vol. 150, Issue 4
Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators
journal, August 2018
- Wang, Degao; Eberhart, Michael S.; Sheridan, Matthew V.
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 34
Dye-sensitized photoelectrochemical water oxidation through a buried junction
journal, June 2018
- Xu, Pengtao; Huang, Tian; Huang, Jianbin
- Proceedings of the National Academy of Sciences, Vol. 115, Issue 27
Inorganic Photochemistry and Solar Energy Harvesting: Current Developments and Challenges to Solar Fuel Production
journal, January 2019
- Sousa, Sinval F.; Souza, Breno L.; Barros, Cristiane L.
- International Journal of Photoenergy, Vol. 2019