Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly
Abstract
The preparation and characterization of new Ru(II) polypyridyl-based chromophore–catalyst assemblies, [(4,4'-PO3H2-bpy)2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)]2+ (1, bpy = 2,2'-bipyridine; 4-Mebpy-4'-epic = 4-(4-methylbipyridin-4'-yl-ethyl)-pyridine; bda = 2,2'-bipyridine-6,6'-dicarboxylate; pic = 4-picoline), and [(bpy)2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)]2+ (1') are described, as is the application of 1 in a dye-sensitized photoelectrosynthesis cell (DSPEC) for solar water splitting. Furthermore, on SnO2/TiO2 core–shell electrodes in a DSPEC configuration with a Pt cathode, the chromophore–catalyst assembly undergoes light-driven water oxidation at pH 5.7 in a 0.1 M acetate buffer, 0.5 M in NaClO4. We observed photocurrents of ~0.85 mA cm–2, with illumination by a 100 mW cm–2 white light source, after 30 s under a 0.1 V vs Ag/AgCl applied bias with a faradaic efficiency for O2 production of 74% measured over a 5 min illumination period.
- Authors:
-
[1];
[2];
- Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States); 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:
- 1349575
- Report Number(s):
- BNL-113712-2017-JA
Journal ID: ISSN 2380-8195; R&D Project: CO026; KC0304030
- Grant/Contract Number:
- SC0012704; SC0001011
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Energy Letters
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Sherman, Benjamin D., Xie, Yan, Sheridan, Matthew V., Wang, Degao, Shaffer, David W., Meyer, Thomas J., and Concepcion, Javier J. Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly. United States: N. p., 2016.
Web. doi:10.1021/acsenergylett.6b00661.
Sherman, Benjamin D., Xie, Yan, Sheridan, Matthew V., Wang, Degao, Shaffer, David W., Meyer, Thomas J., & Concepcion, Javier J. Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly. United States. https://doi.org/10.1021/acsenergylett.6b00661
Sherman, Benjamin D., Xie, Yan, Sheridan, Matthew V., Wang, Degao, Shaffer, David W., Meyer, Thomas J., and Concepcion, Javier J. Fri .
"Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly". United States. https://doi.org/10.1021/acsenergylett.6b00661. https://www.osti.gov/servlets/purl/1349575.
@article{osti_1349575,
title = {Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly},
author = {Sherman, Benjamin D. and Xie, Yan and Sheridan, Matthew V. and Wang, Degao and Shaffer, David W. and Meyer, Thomas J. and Concepcion, Javier J.},
abstractNote = {The preparation and characterization of new Ru(II) polypyridyl-based chromophore–catalyst assemblies, [(4,4'-PO3H2-bpy)2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)]2+ (1, bpy = 2,2'-bipyridine; 4-Mebpy-4'-epic = 4-(4-methylbipyridin-4'-yl-ethyl)-pyridine; bda = 2,2'-bipyridine-6,6'-dicarboxylate; pic = 4-picoline), and [(bpy)2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)]2+ (1') are described, as is the application of 1 in a dye-sensitized photoelectrosynthesis cell (DSPEC) for solar water splitting. Furthermore, on SnO2/TiO2 core–shell electrodes in a DSPEC configuration with a Pt cathode, the chromophore–catalyst assembly undergoes light-driven water oxidation at pH 5.7 in a 0.1 M acetate buffer, 0.5 M in NaClO4. We observed photocurrents of ~0.85 mA cm–2, with illumination by a 100 mW cm–2 white light source, after 30 s under a 0.1 V vs Ag/AgCl applied bias with a faradaic efficiency for O2 production of 74% measured over a 5 min illumination period.},
doi = {10.1021/acsenergylett.6b00661},
journal = {ACS Energy Letters},
number = 1,
volume = 2,
place = {United States},
year = {Fri Dec 09 00:00:00 EST 2016},
month = {Fri Dec 09 00:00:00 EST 2016}
}
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Works referenced in this record:
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
Artificial photosynthesis: Where are we now? Where can we go?
journal, December 2015
- House, Ralph L.; Iha, Neyde Yukie Murakami; Coppo, Rodolfo L.
- Journal of Photochemistry and Photobiology C: Photochemistry Reviews, Vol. 25
Molecular Catalysts for Water Oxidation
journal, July 2015
- Blakemore, James D.; Crabtree, Robert H.; Brudvig, Gary W.
- Chemical Reviews, Vol. 115, Issue 23
Light-Driven Water Splitting with a Molecular Electroassembly-Based Core/Shell Photoanode
journal, July 2015
- Sherman, Benjamin D.; Ashford, Dennis L.; Lapides, Alexander M.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 16
Visible photoelectrochemical water splitting into H 2 and O 2 in a dye-sensitized photoelectrosynthesis cell
journal, April 2015
- Alibabaei, Leila; Sherman, Benjamin D.; Norris, Michael R.
- Proceedings of the National Academy of Sciences, Vol. 112, Issue 19
Light-Induced Redox Reactions in Nanocrystalline Systems
journal, January 1995
- Hagfeldt, Anders.; Graetzel, Michael.
- Chemical Reviews, Vol. 95, Issue 1
A tandem dye-sensitized photoelectrochemical cell for light driven hydrogen production
journal, January 2016
- Sherman, Benjamin D.; Bergkamp, Jesse J.; Brown, Chelsea L.
- Energy & Environmental Science, Vol. 9, Issue 5
Highly efficient water splitting by a dual-absorber tandem cell
journal, November 2012
- Brillet, Jeremie; Yum, Jun-Ho; Cornuz, Maurin
- Nature Photonics, Vol. 6, Issue 12
Organic Dye-Sensitized Tandem Photoelectrochemical Cell for Light Driven Total Water Splitting
journal, July 2015
- Li, Fusheng; Fan, Ke; Xu, Bo
- Journal of the American Chemical Society, Vol. 137, Issue 28
New Photovoltaic Devices Based on the Sensitization of p-type Semiconductors: Challenges and Opportunities
journal, August 2010
- Odobel, Fabrice; Le Pleux, Loïc; Pellegrin, Yann
- Accounts of Chemical Research, Vol. 43, Issue 8
Molecular Chromophore–Catalyst Assemblies for Solar Fuel Applications
journal, August 2015
- Ashford, Dennis L.; Gish, Melissa K.; Vannucci, Aaron K.
- Chemical Reviews, Vol. 115, Issue 23
Evaluation of Chromophore and Assembly Design in Light-Driven Water Splitting with a Molecular Water Oxidation Catalyst
journal, June 2016
- Sheridan, Matthew V.; Sherman, Benjamin D.; Coppo, Rodolfo L.
- ACS Energy Letters, Vol. 1, Issue 1
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
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
Modulating Electron Transfer Dynamics at Dye–Semiconductor Interfaces via Self-Assembled Bilayers
journal, February 2015
- Wang, Jamie C.; Murphy, Ian A.; Hanson, Kenneth
- The Journal of Physical Chemistry C, Vol. 119, Issue 7
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
Self-Assembled Bilayer Films of Ruthenium(II)/Polypyridyl Complexes through Layer-by-Layer Deposition on Nanostructured Metal Oxides
journal, November 2012
- Hanson, Kenneth; Torelli, Daniel A.; Vannucci, Aaron K.
- Angewandte Chemie International Edition, Vol. 51, Issue 51
Photoinduced Electron Transfer in a Chromophore–Catalyst Assembly Anchored to TiO 2
journal, November 2012
- Ashford, Dennis L.; Song, Wenjing; Concepcion, Javier J.
- Journal of the American Chemical Society, Vol. 134, Issue 46
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
Photochemical H2 production with noble-metal-free molecular devices comprising a porphyrin photosensitizer and a cobaloxime catalyst
journal, January 2009
- Zhang, Pan; Wang, Mei; Li, Caixia
- Chemical Communications, Vol. 46, Issue 46
Impact of Ligand Exchange in Hydrogen Production from Cobaloxime-Containing Photocatalytic Systems
journal, November 2011
- McCormick, Theresa M.; Han, Zhiji; Weinberg, David J.
- Inorganic Chemistry, Vol. 50, Issue 21
Ultrafast photodriven intramolecular electron transfer from an iridium-based water-oxidation catalyst to perylene diimide derivatives
journal, May 2012
- Vagnini, M. T.; Smeigh, A. L.; Blakemore, J. D.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 39
Catalytic and Surface-Electrocatalytic Water Oxidation by Redox Mediator-Catalyst Assemblies
journal, November 2009
- Concepcion, Javier J.; Jurss, Jonah W.; Hoertz, Paul G.
- Angewandte Chemie International Edition, Vol. 48, Issue 50
Highly Efficient Bioinspired Molecular Ru Water Oxidation Catalysts with Negatively Charged Backbone Ligands
journal, June 2015
- Duan, Lele; Wang, Lei; Li, Fusheng
- Accounts of Chemical Research, Vol. 48, Issue 7
Artificial photosynthesis – functional devices for light driven water splitting with photoactive anodes based on molecular catalysts
journal, January 2014
- Gao, Yan; Zhang, Linlin; Ding, Xin
- Physical Chemistry Chemical Physics, Vol. 16, Issue 24
A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II
journal, March 2012
- Duan, Lele; Bozoglian, Fernando; Mandal, Sukanta
- Nature Chemistry, Vol. 4, Issue 5
Insights into Ru-Based Molecular Water Oxidation Catalysts: Electronic and Noncovalent-Interaction Effects on Their Catalytic Activities
journal, June 2013
- Duan, Lele; Wang, Lei; Inge, A. Ken
- Inorganic Chemistry, Vol. 52, Issue 14
Charge Recombination Dynamics in Sensitized SnO 2 /TiO 2 Core/Shell Photoanodes
journal, December 2015
- Knauf, Robin R.; Kalanyan, Berç; Parsons, Gregory N.
- The Journal of Physical Chemistry C, Vol. 119, Issue 51
Ultrafast Electron Injection Dynamics of Photoanodes for Water-Splitting Dye-Sensitized Photoelectrochemical Cells
journal, March 2016
- Swierk, John R.; McCool, Nicholas S.; Nemes, Coleen T.
- The Journal of Physical Chemistry C, Vol. 120, Issue 11
Photochemical, Electrochemical, and Photoelectrochemical Water Oxidation Catalyzed by Water-Soluble Mononuclear Ruthenium Complexes
journal, September 2014
- Li, Ting-Ting; Zhao, Wei-Liang; Chen, Yong
- Chemistry - A European Journal, Vol. 20, Issue 43
Two Electrode Collector–Generator Method for the Detection of Electrochemically or Photoelectrochemically Produced O 2
journal, July 2016
- Sherman, Benjamin D.; Sheridan, Matthew V.; Dares, Christopher J.
- Analytical Chemistry, Vol. 88, Issue 14
Electron Transfer Mediator Effects in the Oxidative Activation of a Ruthenium Dicarboxylate Water Oxidation Catalyst
journal, June 2015
- Sheridan, Matthew V.; Sherman, Benjamin D.; Fang, Zhen
- ACS Catalysis, Vol. 5, Issue 7
Analysis of Homogeneous Water Oxidation Catalysis with Collector–Generator Cells
journal, November 2015
- Sherman, Benjamin D.; Sheridan, Matthew V.; Wee, Kyung-Ryang
- Inorganic Chemistry, Vol. 55, Issue 2
Electro-assembly of a Chromophore-Catalyst Bilayer for Water Oxidation and Photocatalytic Water Splitting
journal, February 2015
- Ashford, Dennis L.; Sherman, Benjamin D.; Binstead, Robert A.
- Angewandte Chemie, Vol. 127, Issue 16
Electron Transfer Mediator Effects in Water Oxidation Catalysis by Solution and Surface-Bound Ruthenium Bpy-Dicarboxylate Complexes
journal, October 2015
- Sheridan, Matthew V.; Sherman, Benjamin D.; Marquard, Seth L.
- The Journal of Physical Chemistry C, Vol. 119, Issue 45
Works referencing / citing this record:
A Noble-Metal-Free Heterogeneous Photosensitizer-Relay Catalyst Triad That Catalyzes Water Oxidation under Visible Light
journal, December 2018
- Ulusoy Ghobadi, T. Gamze; Akhuseyin Yildiz, Elif; Buyuktemiz, Muhammed
- Angewandte Chemie, Vol. 130, Issue 52
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
Excited-State Dynamics of [Ru(bpy) 3 ] 2+ Thin Films on Sensitized TiO 2 and ZrO 2
journal, February 2019
- Leandri, Valentina; Liu, Peng; Sadollahkhani, Azar
- ChemPhysChem, Vol. 20, Issue 4
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
Production of solar chemicals: gaining selectivity with hybrid molecule/semiconductor assemblies
journal, January 2018
- Hennessey, Seán; Farràs, Pau
- Chemical Communications, Vol. 54, Issue 50
Directly Photoexcited Oxides for Photoelectrochemical Water Splitting
journal, September 2019
- Pan, Linfeng; Vlachopoulos, Nick; Hagfeldt, Anders
- ChemSusChem, Vol. 12, Issue 19
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
The Role of Antireflective Coating CYTOP, Immersion Oil, and Sensitizer Selection in Fabricating a 2.3 V, 10% Power Conversion Efficiency SSM‐DSC Device
journal, February 2019
- Cheema, Hammad; Delcamp, Jared H.
- Advanced Energy Materials, Vol. 9, Issue 15
Cooperative silanetriolate-carboxylate sensitiser anchoring for outstanding stability and improved performance of dye-sensitised photoelectrodes
journal, January 2018
- Fournier, Maxime; Hoogeveen, Dijon A.; Bonke, Shannon A.
- Sustainable Energy & Fuels, Vol. 2, Issue 8
Early photophysical events of a ruthenium( ii ) molecular dyad capable of performing photochemical water oxidation and of its model compounds
journal, January 2019
- Nastasi, Francesco; Santoro, Antonio; Serroni, Scolastica
- Photochemical & Photobiological Sciences, Vol. 18, Issue 9
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 photoelectrolysis cells
journal, January 2019
- Yun, Sining; Vlachopoulos, Nick; Qurashi, Ahsanulhaq
- Chemical Society Reviews, Vol. 48, Issue 14
Electronic structure and optical properties of isolated and TiO 2 ‐grafted free base porphyrins for water oxidation: A challenging test case for DFT and TD‐DFT
journal, July 2019
- Daoudi, Syrine; Semmeq, Abderrahmane; Badawi, Michael
- Journal of Computational Chemistry, Vol. 40, Issue 29
Visible light-driven water oxidation with a ruthenium sensitizer and a cobalt-based catalyst connected with a polymeric platform
journal, January 2019
- Kap, Zeynep; Karadas, Ferdi
- Faraday Discussions, Vol. 215
A Noble‐Metal‐Free Heterogeneous Photosensitizer‐Relay Catalyst Triad That Catalyzes Water Oxidation under Visible Light
journal, November 2018
- Ulusoy Ghobadi, T. Gamze; Akhuseyin Yildiz, Elif; Buyuktemiz, Muhammed
- Angewandte Chemie International Edition, Vol. 57, Issue 52