Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis

Wang, Degao; Marquard, Seth L.; Troian-Gautier, Ludovic; Sheridan, Matthew V.; Sherman, Benjamin D.; Wang, Ying; Eberhart, Michael S.; Farnum, Byron H.; Dares, Christopher J.; Meyer, Thomas J.

doi:10.1021/jacs.7b10809

Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis

Journal Article · Tue Jan 02 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b10809· OSTI ID:1470086

Wang, Degao ^[1]; Marquard, Seth L. ^[1]; ^[1]; ^[1]; ^[1]; Wang, Ying ^[1]; ^[1]; Farnum, Byron H. ^[1]; ^[2]; ^[1]

Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Florida Intl Univ., Miami, FL (United States). Dept. of Chemistry and Biochemistry

Water oxidation is a critical step in artificial photosynthesis and provides the protons and electrons used in reduction reactions to make solar fuels. Significant advances have been made in the area of molecular water oxidation catalysts with a notable breakthrough in the development of Ru(II) complexes that use a planar “bda” ligand (bda is 2,2'-bipyridine-6,6'-dicarboxylate). These Ru(II)(bda) complexes show lower overpotentials for driving water oxidation making them ideal for light-driven applications with a suitable chromophore. Nevertheless, synthesis of heterogeneous Ru(II)(bda) complexes remains challenging. We discuss here a new “bottom-up” synthetic method for immobilizing these catalysts at the surface of a photoanode for use in a dye-sensitized photoelectrosynthesis cell (DSPEC). The procedure provides a basis for rapidly screening the role of ligand variations at the catalyst in order to understand the impact on device performance. The best results of a water-oxidation DSPEC photoanode based on this procedure reached 1.4 mA/cm² at pH 7 in 0.1 M [PO₄H₂]-/[PO₄H]_2- solution with minimal loss in catalytic behavior over 30 min, and produced an incident photon to current efficiency (IPCE) of 24.8% at 440 nm.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001011

OSTI ID:: 1470086

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 2 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (43)

Molecular-Scale Interface Engineering of TiO2 Nanocrystals: Improve the Efficiency and Stability of Dye-Sensitized Solar Cells Wang, P.; Zakeeruddin, S. M.; Humphry-Baker, R. Advanced Materials, Vol. 15, Issue 24 https://doi.org/10.1002/adma.200306084	journal	December 2003
Effect of Interfacial Engineering in Solid-State Nanostructured Sb ₂ S ₃ Heterojunction Solar Cells Fukumoto, Takafumi; Moehl, Thomas; Niwa, Yusuke Advanced Energy Materials, Vol. 3, Issue 1 https://doi.org/10.1002/aenm.201200540	journal	September 2012
Supramolecular Approaches to Improve the Performance of Ruthenium-Based Water Oxidation Catalysts Kunz, Valentin; Schmidt, David; Röhr, Merle I. S. Advanced Energy Materials, Vol. 7, Issue 16 https://doi.org/10.1002/aenm.201602939	journal	June 2017
Self-Assembled Bilayer Films of Ruthenium(II)/Polypyridyl Complexes through Layer-by-Layer Deposition on Nanostructured Metal Oxides Hanson, Kenneth; Torelli, Daniel A.; Vannucci, Aaron K. Angewandte Chemie International Edition, Vol. 51, Issue 51 https://doi.org/10.1002/anie.201206882	journal	November 2012
Electro-assembly of a Chromophore-Catalyst Bilayer for Water Oxidation and Photocatalytic Water Splitting Ashford, Dennis L.; Sherman, Benjamin D.; Binstead, Robert A. Angewandte Chemie International Edition, Vol. 54, Issue 16 https://doi.org/10.1002/anie.201410944	journal	February 2015
A Million Turnover Molecular Anode for Catalytic Water Oxidation Creus, Jordi; Matheu, Roc; Peñafiel, Itziar Angewandte Chemie International Edition, Vol. 55, Issue 49 https://doi.org/10.1002/anie.201609167	journal	November 2016
Water splitting dye-sensitized solar cells Xu, Pengtao; McCool, Nicholas S.; Mallouk, Thomas E. Nano Today, Vol. 14 https://doi.org/10.1016/j.nantod.2017.04.009	journal	June 2017
Highly Efficient Bioinspired Molecular Ru Water Oxidation Catalysts with Negatively Charged Backbone Ligands Duan, Lele; Wang, Lei; Li, Fusheng Accounts of Chemical Research, Vol. 48, Issue 7 https://doi.org/10.1021/acs.accounts.5b00149	journal	June 2015
Two Electrode Collector–Generator Method for the Detection of Electrochemically or Photoelectrochemically Produced O ₂ Sherman, Benjamin D.; Sheridan, Matthew V.; Dares, Christopher J. Analytical Chemistry, Vol. 88, Issue 14 https://doi.org/10.1021/acs.analchem.6b00738	journal	July 2016
Molecular Chromophore–Catalyst Assemblies for Solar Fuel Applications Ashford, Dennis L.; Gish, Melissa K.; Vannucci, Aaron K. Chemical Reviews, Vol. 115, Issue 23 https://doi.org/10.1021/acs.chemrev.5b00229	journal	August 2015
Manipulating the Rate-Limiting Step in Water Oxidation Catalysis by Ruthenium Bipyridine–Dicarboxylate Complexes Shaffer, David W.; Xie, Yan; Szalda, David J. Inorganic Chemistry, Vol. 55, Issue 22 https://doi.org/10.1021/acs.inorgchem.6b02193	journal	November 2016
Photodriven Oxidation of Surface-Bound Iridium-Based Molecular Water-Oxidation Catalysts on Perylene-3,4-dicarboximide-Sensitized TiO ₂ Electrodes Protected by an Al ₂ O ₃ Layer Kamire, Rebecca J.; Materna, Kelly L.; Hoffeditz, William L. The Journal of Physical Chemistry C, Vol. 121, Issue 7 https://doi.org/10.1021/acs.jpcc.6b11672	journal	February 2017
Light-Driven Water Splitting with a Molecular Electroassembly-Based Core/Shell Photoanode Sherman, Benjamin D.; Ashford, Dennis L.; Lapides, Alexander M. The Journal of Physical Chemistry Letters, Vol. 6, Issue 16 https://doi.org/10.1021/acs.jpclett.5b01370	journal	July 2015
Efficient Light-Driven Oxidation of Alcohols Using an Organic Chromophore–Catalyst Assembly Anchored to TiO ₂ Pho, Toan V.; Sheridan, Matthew V.; Morseth, Zachary A. ACS Applied Materials & Interfaces, Vol. 8, Issue 14 https://doi.org/10.1021/acsami.6b00932	journal	March 2016
Inner Layer Control of Performance in a Dye-Sensitized Photoelectrosynthesis Cell Wang, Degao; Farnum, Byron H.; Sheridan, Matthew V. ACS Applied Materials & Interfaces, Vol. 9, Issue 39 https://doi.org/10.1021/acsami.7b00225	journal	March 2017
Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor Materna, Kelly L.; Rudshteyn, Benjamin; Brennan, Bradley J. ACS Catalysis, Vol. 6, Issue 8 https://doi.org/10.1021/acscatal.6b01101	journal	July 2016
Evaluation of Chromophore and Assembly Design in Light-Driven Water Splitting with a Molecular Water Oxidation Catalyst Sheridan, Matthew V.; Sherman, Benjamin D.; Coppo, Rodolfo L. ACS Energy Letters, Vol. 1, Issue 1 https://doi.org/10.1021/acsenergylett.6b00142	journal	June 2016
Chemical approaches to artificial photosynthesis Meyer, Thomas J. Accounts of Chemical Research, Vol. 22, Issue 5 https://doi.org/10.1021/ar00161a001	journal	May 1989
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
Self-Assembled Bilayers on Indium–Tin Oxide (SAB-ITO) Electrodes: A Design for Chromophore–Catalyst Photoanodes Glasson, Christopher R. K.; Song, Wenjing; Ashford, Dennis L. Inorganic Chemistry, Vol. 51, Issue 16 https://doi.org/10.1021/ic300636w	journal	August 2012
Stabilization of a Ruthenium(II) Polypyridyl Dye on Nanocrystalline TiO ₂ by an Electropolymerized Overlayer Lapides, Alexander M.; Ashford, Dennis L.; Hanson, Kenneth Journal of the American Chemical Society, Vol. 135, Issue 41 https://doi.org/10.1021/ja4055977	journal	October 2013
Dye Stabilization and Enhanced Photoelectrode Wettability in Water-Based Dye-Sensitized Solar Cells through Post-assembly Atomic Layer Deposition of TiO ₂ Son, Ho-Jin; Prasittichai, Chaiya; Mondloch, Joseph E. Journal of the American Chemical Society, Vol. 135, Issue 31 https://doi.org/10.1021/ja406538a	journal	July 2013
Photoassisted Overall Water Splitting in a Visible Light-Absorbing Dye-Sensitized Photoelectrochemical Cell Youngblood, W. Justin; Lee, Seung-Hyun Anna; Kobayashi, Yoji Journal of the American Chemical Society, Vol. 131, Issue 3, p. 926-927 https://doi.org/10.1021/ja809108y	journal	January 2009
Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition Wang, Degao; Sheridan, Matthew V.; Shan, Bing Journal of the American Chemical Society, Vol. 139, Issue 41 https://doi.org/10.1021/jacs.7b07216	journal	August 2017
Enhance the Performance of Dye-Sensitized Solar Cells by Co-grafting Amphiphilic Sensitizer and Hexadecylmalonic Acid on TiO ₂ Nanocrystals Wang, Peng; Zakeeruddin, Shaik M.; Comte, Pascal The Journal of Physical Chemistry B, Vol. 107, Issue 51 https://doi.org/10.1021/jp0365965	journal	December 2003
Stabilizing Small Molecules on Metal Oxide Surfaces Using Atomic Layer Deposition Hanson, Kenneth; Losego, Mark D.; Kalanyan, Berç Nano Letters, Vol. 13, Issue 10 https://doi.org/10.1021/nl402416s	journal	September 2013
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
A supramolecular ruthenium macrocycle with high catalytic activity for water oxidation that mechanistically mimics photosystem II Schulze, Marcus; Kunz, Valentin; Frischmann, Peter D. Nature Chemistry, Vol. 8, Issue 6 https://doi.org/10.1038/nchem.2503	journal	May 2016
Self-assembled molecular p/n junctions for applications in dye-sensitized solar energy conversion Farnum, Byron H.; Wee, Kyung-Ryang; Meyer, Thomas J. Nature Chemistry, Vol. 8, Issue 9 https://doi.org/10.1038/nchem.2536	journal	June 2016
A molecular catalyst for water oxidation that binds to metal oxide surfaces Sheehan, Stafford W.; Thomsen, Julianne M.; Hintermair, Ulrich Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7469	journal	March 2015
Dipicolinic acid: a strong anchoring group with tunable redox and spectral behavior for stable dye-sensitized solar cells Gabrielsson, Erik; Tian, Haining; Eriksson, Susanna K. Chemical Communications, Vol. 51, Issue 18 https://doi.org/10.1039/C4CC06432A	journal	January 2015
Water splitting with polyoxometalate-treated photoanodes: enhancing performance through sensitizer design Fielden, John; Sumliner, Jordan M.; Han, Nannan Chemical Science, Vol. 6, Issue 10 https://doi.org/10.1039/C5SC01439E	journal	January 2015
Synthesis, characterization, and water oxidation by a molecular chromophore-catalyst assembly prepared by atomic layer deposition. The “mummy” strategy Lapides, A. M.; Sherman, B. D.; Brennaman, M. K. Chemical Science, Vol. 6, Issue 11 https://doi.org/10.1039/C5SC01752A	journal	January 2015
Visible light-driven water oxidation using a covalently-linked molecular catalyst–sensitizer dyad assembled on a TiO ₂ electrode Yamamoto, Masanori; Wang, Lei; Li, Fusheng Chemical Science, Vol. 7, Issue 2 https://doi.org/10.1039/C5SC03669K	journal	January 2016
Photoelectrochemical hydrogen production in water using a layer-by-layer assembly of a Ru dye and Ni catalyst on NiO Gross, Manuela A.; Creissen, Charles E.; Orchard, Katherine L. Chemical Science, Vol. 7, Issue 8 https://doi.org/10.1039/C6SC00715E	journal	January 2016
Mechanisms of molecular water oxidation in solution and on oxide surfaces Meyer, Thomas J.; Sheridan, Matthew V.; Sherman, Benjamin D. Chemical Society Reviews, Vol. 46, Issue 20 https://doi.org/10.1039/C7CS00465F	journal	January 2017
O–O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O–O radical coupling Shaffer, David W.; Xie, Yan; Concepcion, Javier J. Chemical Society Reviews, Vol. 46, Issue 20 https://doi.org/10.1039/C7CS00542C	journal	January 2017
A visible light water-splitting cell with a photoanode formed by codeposition of a high-potential porphyrin and an iridium water-oxidation catalyst Moore, Gary F.; Blakemore, James D.; Milot, Rebecca L. Energy & Environmental Science, Vol. 4, Issue 7 https://doi.org/10.1039/c1ee01037a	journal	January 2011
Visible light-driven water oxidation—from molecular catalysts to photoelectrochemical cells Duan, Lele; Tong, Lianpeng; Xu, Yunhua Energy & Environmental Science, Vol. 4, Issue 9 https://doi.org/10.1039/c1ee01276b	journal	January 2011
Synthesis of a series of trifluoromethylazoles and determination of pK a of acidic and basic trifluoromethyl heterocycles by 19F NMR spectroscopy Jones, Brian G.; Branch, Sarah K.; Thompson, Andrew S. Journal of the Chemical Society, Perkin Transactions 1, Issue 22 https://doi.org/10.1039/p19960002685	journal	January 1996
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
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
Plasmon-enhanced light-driven water oxidation by a dye-sensitized photoanode Wang, Degao; Sherman, Benjamin D.; Farnum, Byron H. Proceedings of the National Academy of Sciences, Vol. 114, Issue 37 https://doi.org/10.1073/pnas.1708336114	journal	August 2017

Cited By (21)

Hybrid Photoelectrochemical Water Splitting Systems: From Interface Design to System Assembly Niu, Fujun; Wang, Degao; Li, Fei Advanced Energy Materials, Vol. 10, Issue 11 https://doi.org/10.1002/aenm.201900399	journal	June 2019
Vertical Step‐Growth Polymerization Driven by Electrochemical Stimuli from an Electrode Zhang, Jian; Du, Jia; Wang, Jinxin Angewandte Chemie, Vol. 130, Issue 51 https://doi.org/10.1002/ange.201809567	journal	December 2018
Vertical Step‐Growth Polymerization Driven by Electrochemical Stimuli from an Electrode Zhang, Jian; Du, Jia; Wang, Jinxin Angewandte Chemie International Edition, Vol. 57, Issue 51 https://doi.org/10.1002/anie.201809567	journal	December 2018
Organoruthenium (II) complexes featuring pyrazole-linked Schiff base ligands: Crystal structure, DNA/BSA interactions, cytotoxicity and molecular docking: Half-sandwiched ruthenium complexes Pyrazole schiff base ligand K. S., Neethu; Eswaran, Jayanthi; M., Theetharappan Applied Organometallic Chemistry, Vol. 33, Issue 3 https://doi.org/10.1002/aoc.4751	journal	January 2019
Quantum Chemical Study of the Mechanism of Water Oxidation Catalyzed by a Heterotrinuclear Ru ₂ Mn Complex Li, Ying‐Ying; Gimbert, Carolina; Llobet, Antoni ChemSusChem, Vol. 12, Issue 5 https://doi.org/10.1002/cssc.201802395	journal	February 2019
Protected Hematite Nanorod Arrays with Molecular Complex Co-Catalyst for Efficient and Stable Photoelectrochemical Water Oxidation: Protected Hematite Nanorod Arrays with Molecular Complex Co-Catalyst for Efficient and Stable Photoelectrochemical Water Oxidation Chen, Xiangyan; Fu, Yanming; Kong, Tingting European Journal of Inorganic Chemistry, Vol. 2019, Issue 15 https://doi.org/10.1002/ejic.201801200	journal	December 2018
Three dimensional carbon substrate materials for electrolysis of water Zhang, Xinglin; Shao, Jinjun; Huang, Wei Science China Materials, Vol. 61, Issue 9 https://doi.org/10.1007/s40843-018-9295-8	journal	June 2018
The development of molecular water oxidation catalysts Matheu, Roc; Garrido-Barros, Pablo; Gil-Sepulcre, Marcos Nature Reviews Chemistry, Vol. 3, Issue 5 https://doi.org/10.1038/s41570-019-0096-0	journal	April 2019
Angstrom Thick ZnO Passivation Layer to Improve the Photoelectrochemical Water Splitting Performance of a TiO2 Nanowire Photoanode: The Role of Deposition Temperature Ghobadi, Amir; Ghobadi, Turkan Gamze Ulusoy; Karadas, Ferdi Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-34248-3	journal	November 2018
Production of solar chemicals: gaining selectivity with hybrid molecule/semiconductor assemblies Hennessey, Seán; Farràs, Pau Chemical Communications, Vol. 54, Issue 50 https://doi.org/10.1039/c8cc02487a	journal	January 2018
Core–shell structured titanium dioxide nanomaterials for solar energy utilization Li, Wei; Elzatahry, Ahmed; Aldhayan, Dhaifallah Chemical Society Reviews, Vol. 47, Issue 22 https://doi.org/10.1039/c8cs00443a	journal	January 2018
Dinuclear metal complexes: multifunctional properties and applications Li, Guangfu; Zhu, Dongxia; Wang, Xinlong Chemical Society Reviews, Vol. 49, Issue 3 https://doi.org/10.1039/c8cs00660a	journal	January 2020
Artificial photosynthesis: opportunities and challenges of molecular catalysts Zhang, Biaobiao; Sun, Licheng Chemical Society Reviews, Vol. 48, Issue 7 https://doi.org/10.1039/c8cs00897c	journal	January 2019
P4VP–Ru ^II (bda) polyelectrolyte–metal complex as water oxidation catalyst: on the unique slow-diffusion and multi-charge effects of the polyelectrolyte ligand Zheng, Tao; Zhu, Mo; Waqas, Muhammad RSC Advances, Vol. 8, Issue 68 https://doi.org/10.1039/c8ra08012g	journal	January 2018
A donor-chromophore-catalyst assembly for solar CO ₂ reduction Wang, Degao; Wang, Ying; Brady, Matthew D. Chemical Science, Vol. 10, Issue 16 https://doi.org/10.1039/c8sc03316a	journal	January 2019
Electron injection into titanium dioxide by panchromatic dirhodium photosensitizers with low energy red light Xue, Congcong; Sayre, Hannah J.; Turro, Claudia Chemical Communications, Vol. 55, Issue 70 https://doi.org/10.1039/c9cc04677a	journal	January 2019
Improvement of dye-sensitized solar cell performances through introducing europium dye with multiple excitation: dual enhancement in light absorption Zhang, Lingyun; Wang, Xinzhe; Sun, Xuhui New Journal of Chemistry, Vol. 43, Issue 33 https://doi.org/10.1039/c9nj02985k	journal	January 2019
Light-driven water oxidation by a dye-sensitized photoanode with a chromophore/catalyst assembly on a mesoporous double-shell electrode Liu, Qing; Wang, Degao; Shan, Bing The Journal of Chemical Physics, Vol. 150, Issue 4 https://doi.org/10.1063/1.5048780	journal	January 2019
Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators Wang, Degao; Eberhart, Michael S.; Sheridan, Matthew V. Proceedings of the National Academy of Sciences, Vol. 115, Issue 34 https://doi.org/10.1073/pnas.1802903115	journal	August 2018
A stable dye-sensitized photoelectrosynthesis cell mediated by a NiO overlayer for water oxidation Wang, Degao; Niu, Fujun; Mortelliti, Michael J. Proceedings of the National Academy of Sciences, Vol. 117, Issue 23 https://doi.org/10.1073/pnas.1821687116	journal	September 2019
Inorganic Photochemistry and Solar Energy Harvesting: Current Developments and Challenges to Solar Fuel Production Sousa, Sinval F.; Souza, Breno L.; Barros, Cristiane L. International Journal of Photoenergy, Vol. 2019 https://doi.org/10.1155/2019/9624092	journal	January 2019

Similar Records

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

Journal Article · Mon Oct 15 20:00:00 EDT 2018 · Journal of the American Chemical Society · OSTI ID:1566591

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

Journal Article · Sun Apr 05 20:00:00 EDT 2015 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:1210509

Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly

Journal Article · Thu Dec 08 19:00:00 EST 2016 · ACS Energy Letters · OSTI ID:1349575

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (heterogeneous)
catalysis (homogeneous)
charge transport
electrodes - solar
hydrogen and fuel cells
materials and chemistry by design
photosynthesis (natural and artificial)
solar (fuels)
solar (photovoltaic)
synthesis (novel materials)
synthesis (self-assembly)

Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis

Citation Formats

References (43)

Cited By (21)

Similar Records

Related Subjects