Electron Transfer Mediator Effects in the Oxidative Activation of a Ruthenium Dicarboxylate Water Oxidation Catalyst

Sheridan, Matthew V.; Sherman, Benjamin D.; Fang, Zhen; Wee, Kyung-Ryang; Coggins, Michael K.; Meyer, Thomas J.

doi:10.1021/acscatal.5b00720

Title: Electron Transfer Mediator Effects in the Oxidative Activation of a Ruthenium Dicarboxylate Water Oxidation Catalyst

Journal Article · Fri Jun 19 00:00:00 EDT 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b00720· OSTI ID:1194819

Sheridan, Matthew V. ^[1]; Sherman, Benjamin D. ^[1]; Fang, Zhen ^[1]; Wee, Kyung-Ryang ^[1]; Coggins, Michael K. ^[1]; Meyer, Thomas J. ^[1]

Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States

>The mechanism of electrocatalytic water oxidation by the water oxidation catalyst, ruthenium 2,2'-bipyridine-6,6'-dicarboxylate (bda) bis-isoquinoline (isoq), [Ru(bda)(isoq)₂], 1, at metal oxide electrodes has been investigated. At indium-doped tin oxide (ITO), diminished catalytic currents and increased overpotentials are observed compared to glassy carbon (GC). At pH 7.2 in 0.5 M NaClO₄, catalytic activity is enhanced by the addition of [Ru(bpy)₃]²⁺ (bpy = bipyridine) as a redox mediator. Enhanced catalytic rates are also observed at ITO electrodes derivatized with the surface-bound phosphonic acid derivative [Ru(4,4'-(PO₃H₂)₂bpy)(bpy)₂]²⁺, RuP²⁺. Controlled potential electrolysis with measurement of O₂ at ITO with and without surface-bound RuP²⁺ confirm that water oxidation catalysis occurs. Remarkable rate enhancements are observed with added acetate and phosphate, consistent with an important mechanistic role for atom-proton transfer (APT) in the rate-limiting step as described previously at GC electrodes.

View Journal Article

Cite

Export

Save

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED); University of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001011

OSTI ID:: 1194819

Alternate ID(s):: OSTI ID: 1385928

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Vol. 5 Journal Issue: 7; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 55 works

Citation information provided by
Web of Science

References (34)

Single-Site, Catalytic Water Oxidation on Oxide Surfaces Chen, Zuofeng; Concepcion, Javier J.; Jurss, Jonah W. Journal of the American Chemical Society, Vol. 131, Issue 43, p. 15580-15581 https://doi.org/10.1021/ja906391w	journal	November 2009
Towards A Solar Fuel Device: Light-Driven Water Oxidation Catalyzed by a Supramolecular Assembly Li, Fei; Jiang, Yi; Zhang, Biaobiao Angewandte Chemie International Edition, Vol. 51, Issue 10 https://doi.org/10.1002/anie.201108051	journal	January 2012
Catalytic Water Oxidation by Single-Site Ruthenium Catalysts Concepcion, Javier J.; Jurss, Jonah W.; Norris, Michael R. Inorganic Chemistry, Vol. 49, Issue 4, p. 1277-1279 https://doi.org/10.1021/ic901437e	journal	February 2010
Probing Ligand Effects on O–O Bond Formation of Ru-Catalyzed Water Oxidation: A Computational Survey Kang, Runhua; Chen, Kejuan; Yao, Jiannian Inorganic Chemistry, Vol. 53, Issue 14 https://doi.org/10.1021/ic500008c	journal	June 2014
Base-enhanced catalytic water oxidation by a carboxylate–bipyridine Ru(II) complex Song, Na; Concepcion, Javier J.; Binstead, Robert A. Proceedings of the National Academy of Sciences, Vol. 112, Issue 16 https://doi.org/10.1073/pnas.1500245112	journal	April 2015
Two-Electron, Two-Proton Oxidation of Catechol: Kinetics and Apparent Catalysis Lin, Qianqi; Li, Qian; Batchelor-McAuley, Christopher The Journal of Physical Chemistry C, Vol. 119, Issue 3 https://doi.org/10.1021/jp511414b	journal	January 2015
Redox Mediator Effect on Water Oxidation in a Ruthenium-Based Chromophore–Catalyst Assembly Norris, Michael R.; Concepcion, Javier J.; Harrison, Daniel P. Journal of the American Chemical Society, Vol. 135, Issue 6 https://doi.org/10.1021/ja311645d	journal	January 2013
Control of Catechol and Hydroquinone Electron-Transfer Kinetics on Native and Modified Glassy Carbon Electrodes DuVall, Stacy Hunt; McCreery, Richard L. Analytical Chemistry, Vol. 71, Issue 20 https://doi.org/10.1021/ac990399d	journal	October 1999
Mechanism of water oxidation by [Ru(bda)(L) ₂ ]: the return of the “blue dimer” Concepcion, Javier J.; Zhong, Diane K.; Szalda, David J. Chemical Communications, Vol. 51, Issue 19 https://doi.org/10.1039/C4CC07968J	journal	January 2015
Photocatalytic water oxidation at soft interfaces Hansen, Malte; Li, Fei; Sun, Licheng Chem. Sci., Vol. 5, Issue 7 https://doi.org/10.1039/C4SC01018C	journal	January 2014
Insights into Ru-Based Molecular Water Oxidation Catalysts: Electronic and Noncovalent-Interaction Effects on Their Catalytic Activities Duan, Lele; Wang, Lei; Inge, A. Ken Inorganic Chemistry, Vol. 52, Issue 14 https://doi.org/10.1021/ic302687d	journal	June 2013
Making Oxygen with Ruthenium Complexes Concepcion, Javier J.; Jurss, Jonah W.; Brennaman, M. Kyle Accounts of Chemical Research, Vol. 42, Issue 12 https://doi.org/10.1021/ar9001526	journal	December 2009
Measurement of rates of electron transfer between tris(2,2'-bipyridine)ruthenium(3+) and tris(1,10-phenanthroline)iron(2+) ions and between tris(1,10-phenanthroline)ruthenium(3+) and tris(2,2'-bipyridine)ruthenium(2+) ions by differential excitation flash photolysis Young, Roger C.; Keene, F. Richard; Meyer, Thomas J. Journal of the American Chemical Society, Vol. 99, Issue 8 https://doi.org/10.1021/ja00450a011	journal	April 1977
Concerted O atom-proton transfer in the O--O bond forming step in water oxidation Chen, Z.; Concepcion, J. J.; Hu, X. Proceedings of the National Academy of Sciences, Vol. 107, Issue 16, p. 7225-7229 https://doi.org/10.1073/pnas.1001132107	journal	April 2010
Artificial photosynthesis – functional devices for light driven water splitting with photoactive anodes based on molecular catalysts Gao, Yan; Zhang, Linlin; Ding, Xin Physical Chemistry Chemical Physics, Vol. 16, Issue 24 https://doi.org/10.1039/c3cp55204g	journal	January 2014
Mechanism of Water Oxidation by Single-Site Ruthenium Complex Catalysts Concepcion, Javier J.; Tsai, Ming-Kang; Muckerman, James T. Journal of the American Chemical Society, Vol. 132, Issue 5, p. 1545-1557 https://doi.org/10.1021/ja904906v	journal	February 2010
Surface Activation of Electrocatalysis at Oxide Electrodes. Concerted Electron−Proton Transfer Gagliardi, Christopher J.; Jurss, Jonah W.; Thorp, H. Holden Inorganic Chemistry, Vol. 50, Issue 6 https://doi.org/10.1021/ic102524f	journal	March 2011
Cooperative effects in homogenous water oxidation catalysis by mononuclear ruthenium complexes Mulyana, Yanyan; Keene, F. Richard; Spiccia, Leone Dalton Trans., Vol. 43, Issue 18 https://doi.org/10.1039/C4DT00629A	journal	January 2014
Crossing the divide between homogeneous and heterogeneous catalysis in water oxidation Vannucci, A. K.; Alibabaei, L.; Losego, M. D. Proceedings of the National Academy of Sciences, Vol. 110, Issue 52 https://doi.org/10.1073/pnas.1319832110	journal	November 2013
Three Distinct Redox States of an Oxo-Bridged Dinuclear Ruthenium Complex Yoshida, Masaki; Kondo, Mio; Nakamura, Toshikazu Angewandte Chemie International Edition, Vol. 53, Issue 43 https://doi.org/10.1002/anie.201406443	journal	September 2014
Visible Light-Driven Water Splitting in Photoelectrochemical Cells with Supramolecular Catalysts on Photoanodes Ding, Xin; Gao, Yan; Zhang, Linlin ACS Catalysis, Vol. 4, Issue 7 https://doi.org/10.1021/cs500518k	journal	May 2014
Isolated Seven-Coordinate Ru(IV) Dimer Complex with [HOHOH] ⁻ Bridging Ligand as an Intermediate for Catalytic Water Oxidation Duan, Lele; Fischer, Andreas; Xu, Yunhua Journal of the American Chemical Society, Vol. 131, Issue 30 https://doi.org/10.1021/ja9034686	journal	August 2009
Visible Light Driven Water Splitting in a Molecular Device with Unprecedentedly High Photocurrent Density Gao, Yan; Ding, Xin; Liu, Jianhui Journal of the American Chemical Society, Vol. 135, Issue 11 https://doi.org/10.1021/ja400402d	journal	March 2013
Synthesis of Phosphonic Acid Derivatized Bipyridine Ligands and Their Ruthenium Complexes Norris, Michael R.; Concepcion, Javier J.; Glasson, Christopher R. K. Inorganic Chemistry, Vol. 52, Issue 21 https://doi.org/10.1021/ic4014976	journal	October 2013
Mediator-assisted water oxidation by the ruthenium "blue dimer" cis,cis-[(bpy)2(H2O)RuORu(OH2)(bpy)2]4+ Concepcion, J. J.; Jurss, J. W.; Templeton, J. L. Proceedings of the National Academy of Sciences, Vol. 105, Issue 46 https://doi.org/10.1073/pnas.0807153105	journal	November 2008
Visible Light-Driven Water Oxidation by a Molecular Ruthenium Catalyst in Homogeneous System Duan, Lele; Xu, Yunhua; Zhang, Pan Inorganic Chemistry, Vol. 49, Issue 1 https://doi.org/10.1021/ic9017486	journal	January 2010
A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II Duan, Lele; Bozoglian, Fernando; Mandal, Sukanta Nature Chemistry, Vol. 4, Issue 5 https://doi.org/10.1038/nchem.1301	journal	March 2012
Synthesis and Electrocatalytic Water Oxidation by Electrode-Bound Helical Peptide Chromophore–Catalyst Assemblies Ryan, Derek M.; Coggins, Michael K.; Concepcion, Javier J. Inorganic Chemistry, Vol. 53, Issue 15 https://doi.org/10.1021/ic5011488	journal	July 2014
Surface Catalysis of Water Oxidation by the Blue Ruthenium Dimer Jurss, Jonah W.; Concepcion, Javier C.; Norris, Michael R. Inorganic Chemistry, Vol. 49, Issue 9 https://doi.org/10.1021/ic100469x	journal	May 2010
Highly efficient and robust molecular water oxidation catalysts based on ruthenium complexes Wang, Lei; Duan, Lele; Wang, Ying Chem. Commun., Vol. 50, Issue 85 https://doi.org/10.1039/C4CC05069J	journal	January 2014
Highly efficient and robust molecular ruthenium catalysts for water oxidation Duan, L.; Araujo, C. M.; Ahlquist, M. S. G. Proceedings of the National Academy of Sciences, Vol. 109, Issue 39 https://doi.org/10.1073/pnas.1118347109	journal	July 2012
Mechanisms of Water Oxidation from the Blue Dimer to Photosystem II Liu, Feng; Concepcion, Javier J.; Jurss, Jonah W. Inorganic Chemistry, Vol. 47, Issue 6 https://doi.org/10.1021/ic701249s	journal	March 2008
Promoting the Activity of Catalysts for the Oxidation of Water with Bridged Dinuclear Ruthenium Complexes Jiang, Yi; Li, Fei; Zhang, Biaobiao Angewandte Chemie International Edition, Vol. 52, Issue 12 https://doi.org/10.1002/anie.201209045	journal	February 2013
One-Electron Activation of Water Oxidation Catalysis Tamaki, Yusuke; Vannucci, Aaron K.; Dares, Christopher J. Journal of the American Chemical Society, Vol. 136, Issue 19 https://doi.org/10.1021/ja502637s	journal	May 2014

Similar Records

Base-enhanced catalytic water oxidation by a carboxylate–bipyridine Ru(II) complex

Journal Article · Mon Apr 06 00:00:00 EDT 2015 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:1194819

Song, Na; Concepcion, Javier J.; Binstead, Robert A.; +5 more

A Molecular Silane-Derivatized Ru(II) Catalyst for Photoelectrochemical Water Oxidation

Journal Article · Tue Oct 16 00:00:00 EDT 2018 · Journal of the American Chemical Society · OSTI ID:1194819

Wu, Lei; Eberhart, Michael; Nayak, Animesh; +3 more

Analysis of Homogeneous Water Oxidation Catalysis with Collector–Generator Cells

Journal Article · Thu Nov 12 00:00:00 EST 2015 · Inorganic Chemistry · OSTI ID:1194819

Sherman, Benjamin D.; Sheridan, Matthew V.; Wee, Kyung-Ryang; +6 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
water oxidation
electrocatalysis
electron transfer
polypyridyl ruthenium complexes
water splitting
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)

Title: Electron Transfer Mediator Effects in the Oxidative Activation of a Ruthenium Dicarboxylate Water Oxidation Catalyst

Citation Formats

References (34)

Similar Records

Related Subjects