Light-Driven Water Splitting Mediated by Photogenerated Bromine

Sheridan, Matthew V.; Wang, Ying; Wang, Degao; Troian-Gautier, Ludovic; Dares, Christopher J.; Sherman, Benjamin D.; Meyer, Thomas J.

doi:10.1002/anie.201708879

Title: Light-Driven Water Splitting Mediated by Photogenerated Bromine

Journal Article · Wed Jan 31 00:00:00 EST 2018 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201708879· OSTI ID:1470106

^[1]; Wang, Ying ^[2]; Wang, Degao ^[2];

^[2];

^[1];

^[3];

^[2]

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

Abstract Light‐driven water splitting was achieved using a dye‐sensitized mesoporous oxide film and the oxidation of bromide (Br ⁻ ) to bromine (Br ₂ ) or tribromide (Br ₃ ⁻ ). The chemical oxidant (Br ₂ or Br ₃ ⁻ ) is formed during illumination at the photoanode and used as a sacrificial oxidant to drive a water oxidation catalyst (WOC), here demonstrated using [Ru(bda)(pic) ₂ ], ( 1 ; pic=picoline, bda=2,2′‐bipyridine‐6,6′‐dicarboxylate). The photochemical oxidation of bromide produces a chemical oxidant with a potential of 1.09 V vs. NHE for the Br ₂ /Br ⁻ couple or 1.05 V vs. NHE for the Br ₃ ⁻ /Br ⁻ couple, which is sufficient to drive water oxidation at 1 (Ru ^V/IV ≈1.0 V vs. NHE at pH 5.6). At pH 5.6, using a 0.2 m acetate buffer containing 40 m m LiBr and the [Ru(4,4′‐PO ₃ H ₂ ‐bpy)(bpy) ₂ ] ²⁺ ( RuP ²⁺ , bpy=2,2′‐bipyridine) chromophore dye on a SnO ₂ /TiO ₂ core–shell electrode resulted in a photocurrent density of around 1.2 mA cm ⁻² under approximately 1 Sun illumination and a Faradaic efficiency upon addition of 1 of 77 % for oxygen evolution.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Univ. of North Carolina, Chapel Hill, NC (United States). Energy Frontier Research Center (EFRC) Center for Solar Fuels (UNC)

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

Grant/Contract Number:: SC0001011

OSTI ID:: 1470106

Alternate ID(s):: OSTI ID: 1423382

Journal Information:: Angewandte Chemie (International Edition), Vol. 57, Issue 13; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 25 works

Citation information provided by
Web of Science

References (41)

Effect of iodine concentration on the photovoltaic properties of dye sensitized solar cells for various I2/LiI ratios Mathew, Ambily; Anand, Venu; Rao, G. Mohan Electrochimica Acta, Vol. 87 https://doi.org/10.1016/j.electacta.2012.08.104	journal	January 2013
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
A taxonomy for solar fuels generators Nielander, Adam C.; Shaner, Matthew R.; Papadantonakis, Kimberly M. Energy & Environmental Science, Vol. 8, Issue 1 https://doi.org/10.1039/C4EE02251C	journal	January 2015
Nonaqueous electrocatalytic water oxidation by a surface-bound Ru(bda)(L) ₂ complex Sheridan, Matthew V.; Sherman, Benjamin D.; Wee, Kyung-Ryang Dalton Transactions, Vol. 45, Issue 15 https://doi.org/10.1039/C6DT00408C	journal	January 2016
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
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
Dynamics of Electron Injection in SnO ₂ /TiO ₂ Core/Shell Electrodes for Water-Splitting Dye-Sensitized Photoelectrochemical Cells McCool, Nicholas S.; Swierk, John R.; Nemes, Coleen T. The Journal of Physical Chemistry Letters, Vol. 7, Issue 15 https://doi.org/10.1021/acs.jpclett.6b01528	journal	July 2016
Oxidizing water two ways Meyer, Thomas J. Nature Chemistry, Vol. 3, Issue 10 https://doi.org/10.1038/nchem.1161	journal	September 2011
Aqueous dye-sensitized solar cells Bella, Federico; Gerbaldi, Claudio; Barolo, Claudia Chemical Society Reviews, Vol. 44, Issue 11 https://doi.org/10.1039/C4CS00456F	journal	January 2015
On the electrolysis of aqueous bromide solutions to bromate Cettou, P.; Robertson, P. M.; Ibl, N. Electrochimica Acta, Vol. 29, Issue 7 https://doi.org/10.1016/0013-4686(84)87131-5	journal	July 1984
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
Solar Water Splitting To Generate Hydrogen Fuel: Photothermal Electrochemical Analysis Licht, Stuart The Journal of Physical Chemistry B, Vol. 107, Issue 18 https://doi.org/10.1021/jp026964p	journal	May 2003
Biomimetic and Microbial Approaches to Solar Fuel Generation Magnuson, Ann; Anderlund, Magnus; Johansson, Olof Accounts of Chemical Research, Vol. 42, Issue 12 https://doi.org/10.1021/ar900127h	journal	December 2009
Calculation of pH and Potential E for Bromine Aqueous Solution Michalowski, Tadeusz Journal of Chemical Education, Vol. 71, Issue 7 https://doi.org/10.1021/ed071p560	journal	July 1994
Charge Recombination Dynamics in Sensitized SnO ₂ /TiO ₂ Core/Shell Photoanodes Knauf, Robin R.; Kalanyan, Berç; Parsons, Gregory N. The Journal of Physical Chemistry C, Vol. 119, Issue 51 https://doi.org/10.1021/acs.jpcc.5b10574	journal	December 2015
Kinetic study of the electrochemical processes of the bromine/bromine aqueous system on vitreous carbon electrodes Mastragostino, Marina; Gramellini, Carla Electrochimica Acta, Vol. 30, Issue 3 https://doi.org/10.1016/0013-4686(85)80198-5	journal	March 1985
Photocatalytic Oxidation of Bromide to Bromine Tsai, Kelvin Yun-Da; Chang, I-Jy Inorganic Chemistry, Vol. 56, Issue 2 https://doi.org/10.1021/acs.inorgchem.6b01652	journal	September 2016
The Mechanism of Iodine Reduction by TiO ₂ Electrons and the Kinetics of Recombination in Dye-Sensitized Solar Cells Richards, Caryl E.; Anderson, Assaf Y.; Martiniani, Stefano The Journal of Physical Chemistry Letters, Vol. 3, Issue 15 https://doi.org/10.1021/jz3006755	journal	July 2012
Ultrafast Recombination Dynamics in Dye-Sensitized SnO ₂ /TiO ₂ Core/Shell Films Gish, Melissa K.; Lapides, Alexander M.; Brennaman, M. Kyle The Journal of Physical Chemistry Letters, Vol. 7, Issue 24 https://doi.org/10.1021/acs.jpclett.6b02388	journal	November 2016
Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction McCrory, Charles C. L.; Jung, Suho; Peters, Jonas C. Journal of the American Chemical Society, Vol. 135, Issue 45 https://doi.org/10.1021/ja407115p	journal	October 2013
Site-Selective Passivation of Defects in NiO Solar Photocathodes by Targeted Atomic Deposition Flynn, Cory J.; McCullough, Shannon M.; Oh, EunBi ACS Applied Materials & Interfaces, Vol. 8, Issue 7 https://doi.org/10.1021/acsami.6b01090	journal	February 2016
Interlayer Effects on Oxygen Reduction Kinetics in Porous Electrodes of La _0.5 Sr _0.5 CoO _3-δ Su, Qing; Gong, Wenquan; Yoon, Daeil Journal of The Electrochemical Society, Vol. 161, Issue 4 https://doi.org/10.1149/2.026404jes	journal	January 2014
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
Chloride-assisted catalytic water oxidation Chen, Zuofeng; Concepcion, Javier J.; Song, Na Chemical Communications, Vol. 50, Issue 59 https://doi.org/10.1039/c4cc04071f	journal	January 2014
Triiodide ion formation equilibrium and activity coefficients in aqueous solution Palmer, Donald A.; Ramette, R. W.; Mesmer, R. E. Journal of Solution Chemistry, Vol. 13, Issue 9 https://doi.org/10.1007/BF00650374	journal	September 1984
Characteristics of the Iodide/Triiodide Redox Mediator in Dye-Sensitized Solar Cells Boschloo, Gerrit; Hagfeldt, Anders Accounts of Chemical Research, Vol. 42, Issue 11 https://doi.org/10.1021/ar900138m	journal	November 2009
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
A mechanistic study of the electro-oxidation of bromide in acetonitrile and the room temperature ionic liquid, 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide at platinum electrodes Allen, Gary D.; Buzzeo, Marisa C.; Villagrán, Constanza Journal of Electroanalytical Chemistry, Vol. 575, Issue 2 https://doi.org/10.1016/j.jelechem.2004.09.023	journal	February 2005
Interfacial Recombination Processes in Dye-Sensitized Solar Cells and Methods To Passivate the Interfaces Gregg, Brian A.; Pichot, François; Ferrere, Suzanne The Journal of Physical Chemistry B, Vol. 105, Issue 7 https://doi.org/10.1021/jp003000u	journal	February 2001
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
Research opportunities to advance solar energy utilization Lewis, N. S. Science, Vol. 351, Issue 6271 https://doi.org/10.1126/science.aad1920	journal	January 2016
Rutile TiO ₂ as an Anode Material for Water-Splitting Dye-Sensitized Photoelectrochemical Cells Swierk, John R.; Regan, Kevin P.; Jiang, Jianbing ACS Energy Letters, Vol. 1, Issue 3 https://doi.org/10.1021/acsenergylett.6b00279	journal	August 2016
Oxidation of Bromide to Bromine by Ruthenium(II) Bipyridine-Type Complexes Using the Flash-Quench Technique Tsai, Kelvin Yun-Da; Chang, I-Jy Inorganic Chemistry, Vol. 56, Issue 14 https://doi.org/10.1021/acs.inorgchem.7b01238	journal	June 2017
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
Visible Light Driven Nanosecond Bromide Oxidation by a Ru Complex with Subsequent Br–Br Bond Formation Li, Guocan; Ward, William M.; Meyer, Gerald J. Journal of the American Chemical Society, Vol. 137, Issue 26 https://doi.org/10.1021/jacs.5b04549	journal	June 2015
Molecular Catalysts for Water Oxidation Blakemore, James D.; Crabtree, Robert H.; Brudvig, Gary W. Chemical Reviews, Vol. 115, Issue 23 https://doi.org/10.1021/acs.chemrev.5b00122	journal	July 2015
Use of Bromine and Bromo-Organic Compounds in Organic Synthesis Saikia, Indranirekha; Borah, Arun Jyoti; Phukan, Prodeep Chemical Reviews, Vol. 116, Issue 12 https://doi.org/10.1021/acs.chemrev.5b00400	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
Bromine perchlorate Schack, Carl J.; Christe, Karl O.; Pilipovich, Donald Inorganic Chemistry, Vol. 10, Issue 5 https://doi.org/10.1021/ic50099a045	journal	May 1971
Site-Selective Passivation of Defects in NiO Solar Photocathodes by Targeted Atomic Deposition L., Li,; J. R., McBride,; T. J., Meyer, The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/mt30-nx40	text	January 2016
Base-enhanced catalytic water oxidation by a carboxylate–bipyridine Ru(II) complex J., Meyer, Thomas; K., Coggins, Michael; K., Vannucci, Aaron The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/w0m4-tb12	text	January 2015

Cited By (6)

Constructing Multi‐Stimuli‐Responsive Luminescent Materials through Outer Sphere Electron Transfer in Ion Pairs Ma, Yun; Shen, Liang; She, Pengfei Advanced Optical Materials, Vol. 7, Issue 8 https://doi.org/10.1002/adom.201801657	journal	January 2019
Doping‐Induced Amorphization, Vacancy, and Gradient Energy Band in SnS ₂ Nanosheet Arrays for Improved Photoelectrochemical Water Splitting Meng, Linxing; Wang, Siyu; Cao, Fengren Angewandte Chemie, Vol. 131, Issue 20 https://doi.org/10.1002/ange.201902411	journal	April 2019
Doping‐Induced Amorphization, Vacancy, and Gradient Energy Band in SnS ₂ Nanosheet Arrays for Improved Photoelectrochemical Water Splitting Meng, Linxing; Wang, Siyu; Cao, Fengren Angewandte Chemie International Edition, Vol. 58, Issue 20 https://doi.org/10.1002/anie.201902411	journal	May 2019
Robust, Scalable Synthesis of the Bulky Hagfeldt Donor for Dye‐Sensitized Solar Cells Baumann, Alexandra; Watson, Jonathon; Delcamp, Jared H. ChemSusChem, Vol. 13, Issue 2 https://doi.org/10.1002/cssc.201902349	journal	October 2019
A synergistic LUMO lowering strategy using Lewis acid catalysis in water to enable photoredox catalytic, functionalizing C–C cross-coupling of styrenes Speckmeier, Elisabeth; Fuchs, Patrick J. W.; Zeitler, Kirsten Chemical Science, Vol. 9, Issue 35 https://doi.org/10.1039/c8sc02106f	journal	January 2018
Electronic Properties of Electron-Deficient Zn(II) Porphyrins for HBr Splitting Berardi, Serena; Caramori, Stefano; Benazzi, Elisabetta Applied Sciences, Vol. 9, Issue 13 https://doi.org/10.3390/app9132739	journal	July 2019

Similar Records

Light‐Driven Water Splitting Mediated by Photogenerated Bromine

Journal Article · Mon Mar 19 00:00:00 EDT 2018 · Angewandte Chemie · OSTI ID:1470106

Sheridan, Matthew V.; Wang, Ying; Wang, Degao; +4 more

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

Journal Article · Fri Dec 09 00:00:00 EST 2016 · ACS Energy Letters · OSTI ID:1470106

Sherman, Benjamin D.; Xie, Yan; Sheridan, Matthew V.; +4 more

All-in-One Derivatized Tandem p⁺n-Silicon–SnO₂/TiO₂ Water Splitting Photoelectrochemical Cell

Journal Article · Mon Feb 27 00:00:00 EST 2017 · Nano Letters · OSTI ID:1470106

Sheridan, Matthew V.; Hill, David J.; Sherman, Benjamin D.; +5 more

Related Subjects

25 ENERGY STORAGE
energy storage
photochemistry
photoelectrochemistry
water oxidation
water splitting

Title: Light-Driven Water Splitting Mediated by Photogenerated Bromine

Citation Formats

References (41)

Cited By (6)

Similar Records

Related Subjects