Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II

Wang, Degao; Sampaio, Renato N.; Troian-Gautier, Ludovic; Marquard, Seth L.; Farnum, Byron H.; Sherman, Benjamin D.; Sheridan, Matthew V.; Dares, Christopher J.; Meyer, Gerald J.; Meyer, Thomas J.

doi:10.1021/jacs.9b02548

Title: Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II

Journal Article · Thu Apr 25 00:00:00 EDT 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b02548· OSTI ID:1566599

Wang, Degao ^[1];

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Univ. of North Carolina, Chapel Hill, NC (United States)
Auburn Univ., AL (United States)
Texas Christian Univ., Fort Worth, TX (United States)
Florida International Univ., Miami, FL (United States)

In artificial photosynthesis, the sun drives water splitting into H₂ and O₂ or converts CO₂ into a useful form of carbon. In most schemes, water oxidation is typically the limiting half-reaction. Here, we introduce a molecular approach to the design of a photoanode that incorporates an electron acceptor, a sensitizer, an electron donor, and a water oxidation catalyst in a single molecular assembly. The strategy mimics the key elements in Photosystem II by initiating light-driven water oxidation with integration of a light absorber, an electron acceptor, an electron donor, and a catalyst in a controlled molecular environment on the surface of a conducting oxide electrode. Visible excitation of the assembly results in the appearance of reductive equivalents at the electrode and oxidative equivalents at a catalyst that persist for seconds in aqueous solutions. Steady-state illumination of the assembly with 440 nm light with an applied bias results in photoelectrochemical water oxidation with a per-photon absorbed efficiency of 2.3%. Here, the results are notable in demonstrating that light-driven water oxidation can be carried out at a conductive electrode in a structure with the functional elements of Photosystem II including charge separation and water oxidation.

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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:: 1566599

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 19; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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References (50)

Powering the planet: Chemical challenges in solar energy utilization Lewis, N. S.; Nocera, D. G. Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735 https://doi.org/10.1073/pnas.0603395103	journal	October 2006
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
Oxidizing water two ways Meyer, Thomas J. Nature Chemistry, Vol. 3, Issue 10 https://doi.org/10.1038/nchem.1161	journal	September 2011
Solar Water Splitting Cells Walter, Michael G.; Warren, Emily L.; McKone, James R. Chemical Reviews, Vol. 110, Issue 11, p. 6446-6473 https://doi.org/10.1021/cr1002326	journal	November 2010
Electrochemical Photolysis of Water at a Semiconductor Electrode Fujishima, Akira; Honda, Kenichi Nature, Vol. 238, Issue 5358, p. 37-38 https://doi.org/10.1038/238037a0	journal	July 1972
Amorphous TiO2 coatings stabilize Si, GaAs, and GaP photoanodes for efficient water oxidation Hu, S.; Shaner, M. R.; Beardslee, J. A. Science, Vol. 344, Issue 6187 https://doi.org/10.1126/science.1251428	journal	May 2014
High-Performance Silicon Photoanodes Passivated with Ultrathin Nickel Films for Water Oxidation Kenney, M. J.; Gong, M.; Li, Y. Science, Vol. 342, Issue 6160 https://doi.org/10.1126/science.1241327	journal	November 2013
Semiconductor Nanowires for Artificial Photosynthesis Liu, Chong; Dasgupta, Neil P.; Yang, Peidong Chemistry of Materials, Vol. 26, Issue 1 https://doi.org/10.1021/cm4023198	journal	September 2013
Solar Water Splitting: Progress Using Hematite (α-Fe2O3) Photoelectrodes Sivula, Kevin; Le Formal, Florian; Grätzel, Michael ChemSusChem, Vol. 4, Issue 4 https://doi.org/10.1002/cssc.201000416	journal	March 2011
Light-Harvesting and Photocurrent Generation by Gold Electrodes Modified with Mixed Self-Assembled Monolayers of Boron−Dipyrrin and Ferrocene−Porphyrin−Fullerene Triad Imahori, Hiroshi; Norieda, Hiroyuki; Yamada, Hiroko Journal of the American Chemical Society, Vol. 123, Issue 1 https://doi.org/10.1021/ja002154k	journal	January 2001
Photodriven transmembrane charge separation and electron transfer by a carotenoporphyrin–quinone triad Seta, Patrick; Bienvenue, Elisabeth; Moore, Ana L. Nature, Vol. 316, Issue 6029 https://doi.org/10.1038/316653a0	journal	August 1985
Evolution of reaction center mimics to systems capable of generating solar fuel Sherman, Benjamin D.; Vaughn, Michael D.; Bergkamp, Jesse J. Photosynthesis Research, Vol. 120, Issue 1-2 https://doi.org/10.1007/s11120-013-9795-4	journal	February 2013
Linkage and Solvent Dependence of Photoinduced Electron Transfer in Zincporphyrin-C ₆₀ Dyads Imahori, Hiroshi; Hagiwara, Kiyoshi; Aoki, Masanori Journal of the American Chemical Society, Vol. 118, Issue 47 https://doi.org/10.1021/ja9628415	journal	January 1996
Photoinduced Charge Separation and Charge Recombination to a Triplet State in a Carotene−Porphyrin−Fullerene Triad Liddell, Paul A.; Kuciauskas, Darius; Sumida, John P. Journal of the American Chemical Society, Vol. 119, Issue 6 https://doi.org/10.1021/ja9631054	journal	February 1997
A Charge‐Separated State that Lives for Almost a Second at a Conductive Metal Oxide Interface Sampaio, Renato N.; Troian‐Gautier, Ludovic; Meyer, Gerald J. Angewandte Chemie, Vol. 130, Issue 47 https://doi.org/10.1002/ange.201807627	journal	November 2018
Visible photoelectrochemical water splitting into H ₂ and O ₂ in a dye-sensitized photoelectrosynthesis cell Alibabaei, Leila; Sherman, Benjamin D.; Norris, Michael R. Proceedings of the National Academy of Sciences, Vol. 112, Issue 19 https://doi.org/10.1073/pnas.1506111112	journal	April 2015
Organic Dye-Sensitized Tandem Photoelectrochemical Cell for Light Driven Total Water Splitting Li, Fusheng; Fan, Ke; Xu, Bo Journal of the American Chemical Society, Vol. 137, Issue 28 https://doi.org/10.1021/jacs.5b04856	journal	July 2015
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
A Dye-Sensitized Photoelectrochemical Tandem Cell for Light Driven Hydrogen Production from Water Sherman, Benjamin D.; Sheridan, Matthew V.; Wee, Kyung-Ryang Journal of the American Chemical Society, Vol. 138, Issue 51 https://doi.org/10.1021/jacs.6b10699	journal	December 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
Chemical approaches to artificial photosynthesis Concepcion, J. J.; House, R. L.; Papanikolas, J. M. Proceedings of the National Academy of Sciences, Vol. 109, Issue 39 https://doi.org/10.1073/pnas.1212254109	journal	September 2012
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
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
Solar Fuels via Artificial Photosynthesis Gust, Devens; Moore, Thomas A.; Moore, Ana L. Accounts of Chemical Research, Vol. 42, Issue 12 https://doi.org/10.1021/ar900209b	journal	December 2009
Visible Light Water Splitting Using Dye-Sensitized Oxide Semiconductors Youngblood, W. Justin; Lee, Seung-Hyun Anna; Maeda, Kazuhiko Accounts of Chemical Research, Vol. 42, Issue 12 https://doi.org/10.1021/ar9002398	journal	December 2009
Generation of Long-Lived Redox Equivalents in Self-Assembled Bilayer Structures on Metal Oxide Electrodes Shan, Bing; Farnum, Byron H.; Wee, Kyung-Ryang The Journal of Physical Chemistry C, Vol. 121, Issue 11 https://doi.org/10.1021/acs.jpcc.6b12416	journal	March 2017
Modulating Hole Transport in Multilayered Photocathodes with Derivatized p-Type Nickel Oxide and Molecular Assemblies for Solar-Driven Water Splitting Shan, Bing; Sherman, Benjamin D.; Klug, Christina M. The Journal of Physical Chemistry Letters, Vol. 8, Issue 18 https://doi.org/10.1021/acs.jpclett.7b01911	journal	August 2017
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 Journal of the American Chemical Society, Vol. 140, Issue 2 https://doi.org/10.1021/jacs.7b10809	journal	January 2018
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
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
Direct photoactivation of a nickel-based, water-reduction photocathode by a highly conjugated supramolecular chromophore Shan, Bing; Nayak, Animesh; N. Sampaio, Renato Energy & Environmental Science, Vol. 11, Issue 2 https://doi.org/10.1039/C7EE03115G	journal	January 2018
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
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, Vol. 124, Issue 51 https://doi.org/10.1002/ange.201206882	journal	November 2012
Synthesis and photophysical characterization of porphyrin and porphyrin–Ru(ii) polypyridyl chromophore–catalyst assemblies on mesoporous metal oxides Nayak, Animesh; Knauf, Robin R.; Hanson, Kenneth Chemical Science, Vol. 5, Issue 8 https://doi.org/10.1039/c4sc00875h	journal	January 2014
The Possible Role of Proton-Coupled Electron Transfer (PCET) in Water Oxidation by Photosystem II Meyer, Thomas J.; Huynh, My Hang V.; Thorp, H. Holden Angewandte Chemie International Edition, Vol. 46, Issue 28 https://doi.org/10.1002/anie.200600917	journal	July 2007
Proton-coupled electron transfer of tyrosines in Photosystem II and model systems for artificial photosynthesis: the role of a redox-active link between catalyst and photosensitizer Hammarström, Leif; Styring, Stenbjörn Energy & Environmental Science, Vol. 4, Issue 7 https://doi.org/10.1039/c1ee01348c	journal	January 2011
Water-Splitting Chemistry of Photosystem II McEvoy, James P.; Brudvig, Gary W. Chemical Reviews, Vol. 106, Issue 11 https://doi.org/10.1021/cr0204294	journal	November 2006
Mimicking the electron transfer chain in photosystem II with a molecular triad thermodynamically capable of water oxidation Megiatto, J. D.; Antoniuk-Pablant, A.; Sherman, B. D. Proceedings of the National Academy of Sciences, Vol. 109, Issue 39 https://doi.org/10.1073/pnas.1118348109	journal	May 2012
Improving the efficiency of water splitting in dye-sensitized solar cells by using a biomimetic electron transfer mediator Zhao, Y.; Swierk, J. R.; Megiatto, J. D. Proceedings of the National Academy of Sciences, Vol. 109, Issue 39 https://doi.org/10.1073/pnas.1118339109	journal	April 2012
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
Optical Intramolecular Electron Transfer in Opposite Directions through the Same Bridge That Follows Different Pathways Piechota, Eric J.; Troian-Gautier, Ludovic; Sampaio, Renato N. Journal of the American Chemical Society, Vol. 140, Issue 23 https://doi.org/10.1021/jacs.8b02715	journal	May 2018
Thin Film Actinometers for Transient Absorption Spectroscopy: Applications to Dye-Sensitized Solar Cells Bergeron, Bryan V.; Kelly, Craig A.; Meyer, Gerald J. Langmuir, Vol. 19, Issue 20 https://doi.org/10.1021/la035053j	journal	September 2003
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
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
Ultrafast Electrochromic Windows Based on Redox-Chromophore Modified Nanostructured Semiconducting and Conducting Films Cummins, David; Boschloo, Gerrit; Ryan, Michael The Journal of Physical Chemistry B, Vol. 104, Issue 48 https://doi.org/10.1021/jp001763b	journal	December 2000
Ultrafast, Light-Induced Electron Transfer in a Perylene Diimide Chromophore-Donor Assembly on TiO ₂ Brennaman, M. Kyle; Norris, Michael R.; Gish, Melissa K. The Journal of Physical Chemistry Letters, Vol. 6, Issue 23 https://doi.org/10.1021/acs.jpclett.5b02194	journal	November 2015
Kinetics teach that electronic coupling lowers the free-energy change that accompanies electron transfer Sampaio, Renato N.; Piechota, Eric J.; Troian-Gautier, Ludovic Proceedings of the National Academy of Sciences, Vol. 115, Issue 28 https://doi.org/10.1073/pnas.1722401115	journal	June 2018
Kinetic pathway for interfacial electron transfer from a semiconductor to a molecule Hu, Ke; Blair, Amber D.; Piechota, Eric J. Nature Chemistry, Vol. 8, Issue 9 https://doi.org/10.1038/nchem.2549	journal	June 2016
A High-Valent Metal-Oxo Species Produced by Photoinduced One-Electron, Two-Proton Transfer Reactivity Hu, Ke; Sampaio, Renato N.; Marquard, Seth L. Inorganic Chemistry, Vol. 57, Issue 1 https://doi.org/10.1021/acs.inorgchem.7b02758	journal	December 2017
Non-symmetrical dielectric relaxation behaviour arising from a simple empirical decay function Williams, Graham; Watts, David C. Transactions of the Faraday Society, Vol. 66 https://doi.org/10.1039/tf9706600080	journal	January 1970

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (homogeneous)
catalysis (heterogeneous)
electrocatalysis
solar (fuels)
photosynthesis (natural and artificial)
defects
charge transport
materials and chemistry by design
mesostructured materials
synthesis (novel materials)
synthesis (self-assembly)
charge transfer
electrodes
catalysts
oxidation water oxidation

Title: Molecular Photoelectrode for Water Oxidation Inspired by Photosystem II

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References (50)

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