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Title: Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators

Abstract

Stabilized photoanodes for light-driven water oxidation have been prepared on nanoparticle core/shell electrodes with surface-stabilized donor–acceptor chromophores, a water oxidation catalyst, and an electron-transfer mediator. Here, for the electrode, fluorine-doped tin oxide FTO|SnO2/TiO2|-Org1-|1.1 nm Al2O3|-RuP2+-WOC (water oxidation catalyst) with Org1 (1-cyano-2-(4-(diphenylamino)phenyl)vinyl)phosphonic acid), the mediator RuP2+([Ru(4,4-(PO3H2)2-2,2-bipyridine)(2,2-bipyridine)2]2+), and the WOC, Ru(bda)(py(CH2)(3or10)P(O3H)2)2(bda is 2,2-bipyridine-6,6-dicarboxylate with x = 3 or 10), solar excitation resulted in photocurrents of ~500 µA/cm2and quantitative O2evolution at pH 4.65. Related results were obtained for other Ru(II) polypyridyl mediators. For the organic dye PP (5-(4-(dihydroxyphosphoryl)phenyl)-10,15,20-Tris(mesityl)porphyrin), solar water oxidation occurred with a driving force near 0 V.

Authors:
 [1];  [1];  [1];  [2]; ORCiD logo [3];  [1];  [1];  [1]; ORCiD logo [4];  [1]
  1. Univ. of North Carolina, Chapel Hill, NC (United States)
  2. Fudan Univ., Shanghai (People's Republic of China)
  3. Univ. of North Carolina, Chapel Hill, NC (United States); Texas Christian Univ., Fort Worth, TX (United States)
  4. Florida International Univ., Miami, FL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED); Univ. of North Carolina, Chapel Hill, NC (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1540291
Grant/Contract Number:  
SC0001011
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 115; Journal Issue: 34; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Science & Technology; Other Topics; core/shell; water oxidation; electron-transfer mediator; DSPEC; organic dye

Citation Formats

Wang, Degao, Eberhart, Michael S., Sheridan, Matthew V., Hu, Ke, Sherman, Benjamin D., Nayak, Animesh, Wang, Ying, Marquard, Seth L., Dares, Christopher J., and Meyer, Thomas J. Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators. United States: N. p., 2018. Web. doi:10.1073/pnas.1802903115.
Wang, Degao, Eberhart, Michael S., Sheridan, Matthew V., Hu, Ke, Sherman, Benjamin D., Nayak, Animesh, Wang, Ying, Marquard, Seth L., Dares, Christopher J., & Meyer, Thomas J. Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators. United States. doi:https://doi.org/10.1073/pnas.1802903115
Wang, Degao, Eberhart, Michael S., Sheridan, Matthew V., Hu, Ke, Sherman, Benjamin D., Nayak, Animesh, Wang, Ying, Marquard, Seth L., Dares, Christopher J., and Meyer, Thomas J. Mon . "Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators". United States. doi:https://doi.org/10.1073/pnas.1802903115. https://www.osti.gov/servlets/purl/1540291.
@article{osti_1540291,
title = {Stabilized photoanodes for water oxidation by integration of organic dyes, water oxidation catalysts, and electron-transfer mediators},
author = {Wang, Degao and Eberhart, Michael S. and Sheridan, Matthew V. and Hu, Ke and Sherman, Benjamin D. and Nayak, Animesh and Wang, Ying and Marquard, Seth L. and Dares, Christopher J. and Meyer, Thomas J.},
abstractNote = {Stabilized photoanodes for light-driven water oxidation have been prepared on nanoparticle core/shell electrodes with surface-stabilized donor–acceptor chromophores, a water oxidation catalyst, and an electron-transfer mediator. Here, for the electrode, fluorine-doped tin oxide FTO|SnO2/TiO2|-Org1-|1.1 nm Al2O3|-RuP2+-WOC (water oxidation catalyst) with Org1 (1-cyano-2-(4-(diphenylamino)phenyl)vinyl)phosphonic acid), the mediator RuP2+([Ru(4,4-(PO3H2)2-2,2-bipyridine)(2,2-bipyridine)2]2+), and the WOC, Ru(bda)(py(CH2)(3or10)P(O3H)2)2(bda is 2,2-bipyridine-6,6-dicarboxylate with x = 3 or 10), solar excitation resulted in photocurrents of ~500 µA/cm2and quantitative O2evolution at pH 4.65. Related results were obtained for other Ru(II) polypyridyl mediators. For the organic dye PP (5-(4-(dihydroxyphosphoryl)phenyl)-10,15,20-Tris(mesityl)porphyrin), solar water oxidation occurred with a driving force near 0 V.},
doi = {10.1073/pnas.1802903115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 34,
volume = 115,
place = {United States},
year = {2018},
month = {8}
}

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