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'-PO 3H 2-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 SnO 2/TiO 2 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 NaClO 4. 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 O 2 production of 74% measured over a 5 min illumination period.
- Authors:
-
- 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:
- Journal Article: 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},
url = {https://www.osti.gov/biblio/1349575},
journal = {ACS Energy Letters},
issn = {2380-8195},
number = 1,
volume = 2,
place = {United States},
year = {2016},
month = {12}
}
Web of Science
Works referencing / citing this record:
Noncovalent immobilization and surface characterization of lanthanide complexes on carbon electrodes
journal, January 2017
- Lionetti, Davide; Day, Victor W.; Blakemore, James D.
- Dalton Transactions, Vol. 46, Issue 35
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
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
Noncovalent immobilization and surface characterization of lanthanide complexes on carbon electrodes
journal, January 2017
- Lionetti, Davide; Day, Victor W.; Blakemore, James D.
- Dalton Transactions, Vol. 46, Issue 35
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
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
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
Directly Photoexcited Oxides for Photoelectrochemical Water Splitting
journal, September 2019
- Pan, Linfeng; Vlachopoulos, Nick; Hagfeldt, Anders
- ChemSusChem, Vol. 12, Issue 19
O–O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O–O radical coupling
journal, January 2017
- Shaffer, David W.; Xie, Yan; Concepcion, Javier J.
- Chemical Society Reviews, Vol. 46, Issue 20
Production of solar chemicals: gaining selectivity with hybrid molecule/semiconductor assemblies
journal, January 2018
- Hennessey, Seán; Farràs, Pau
- Chemical Communications, Vol. 54, Issue 50
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
Artificial photosynthesis: opportunities and challenges of molecular catalysts
journal, January 2019
- Zhang, Biaobiao; Sun, Licheng
- Chemical Society Reviews, Vol. 48, Issue 7
Dye sensitized photoelectrolysis cells
journal, January 2019
- Yun, Sining; Vlachopoulos, Nick; Qurashi, Ahsanulhaq
- Chemical Society Reviews, Vol. 48, Issue 14
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
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
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
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
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
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