Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells
Abstract
Solar fuel generation requires the efficient capture and conversion of visible light. In both natural and artificial systems, molecular sensitizers can be tuned to capture, convert, and transfer visible light energy. We demonstrate that a series of metal-free porphyrins can drive photoelectrochemical water splitting under broadband and red light (λ > 590 nm) illumination in a dye-sensitized TiO2 solar cell. Here, we report the synthesis, spectral, and electrochemical properties of the sensitizers. Despite slow recombination of photoinjected electrons with oxidized porphyrins, photocurrents are low because of low injection yields and slow electron self-exchange between oxidized porphyrins. As a result, the free-base porphyrins are stable under conditions of water photoelectrolysis and in some cases photovoltages in excess of 1 V are observed.
- Authors:
-
- Departments of aChemistry and
- Department of Chemistry and Biochemistry and Center for Bio-Inspired Solar Fuel Production, Arizona State University, Tempe, AZ 85287
- Departments of aChemistry and, Biochemistry and Molecular Biology, Pennsylvania State University, University Park, PA 16802, and
- Publication Date:
- Research Org.:
- Arizona State Univ., Tempe, AZ (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Solar Fuel Production (BISfuel)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1235499
- Alternate Identifier(s):
- OSTI ID: 1348410
- Grant/Contract Number:
- FG02-07ER15911; SC0001016; DGE1255832; ECS-0335765
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 112 Journal Issue: 6; Journal ID: ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; artificial photosynthesis; metal-free porphyrins; photoelectrochemical; visible light; water-splitting
Citation Formats
Swierk, John R., Méndez-Hernández, Dalvin D., McCool, Nicholas S., Liddell, Paul, Terazono, Yuichi, Pahk, Ian, Tomlin, John J., Oster, Nolan V., Moore, Thomas A., Moore, Ana L., Gust, Devens, and Mallouk, Thomas E. Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells. United States: N. p., 2015.
Web. doi:10.1073/pnas.1414901112.
Swierk, John R., Méndez-Hernández, Dalvin D., McCool, Nicholas S., Liddell, Paul, Terazono, Yuichi, Pahk, Ian, Tomlin, John J., Oster, Nolan V., Moore, Thomas A., Moore, Ana L., Gust, Devens, & Mallouk, Thomas E. Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells. United States. https://doi.org/10.1073/pnas.1414901112
Swierk, John R., Méndez-Hernández, Dalvin D., McCool, Nicholas S., Liddell, Paul, Terazono, Yuichi, Pahk, Ian, Tomlin, John J., Oster, Nolan V., Moore, Thomas A., Moore, Ana L., Gust, Devens, and Mallouk, Thomas E. Mon .
"Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells". United States. https://doi.org/10.1073/pnas.1414901112.
@article{osti_1235499,
title = {Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells},
author = {Swierk, John R. and Méndez-Hernández, Dalvin D. and McCool, Nicholas S. and Liddell, Paul and Terazono, Yuichi and Pahk, Ian and Tomlin, John J. and Oster, Nolan V. and Moore, Thomas A. and Moore, Ana L. and Gust, Devens and Mallouk, Thomas E.},
abstractNote = {Solar fuel generation requires the efficient capture and conversion of visible light. In both natural and artificial systems, molecular sensitizers can be tuned to capture, convert, and transfer visible light energy. We demonstrate that a series of metal-free porphyrins can drive photoelectrochemical water splitting under broadband and red light (λ > 590 nm) illumination in a dye-sensitized TiO2 solar cell. Here, we report the synthesis, spectral, and electrochemical properties of the sensitizers. Despite slow recombination of photoinjected electrons with oxidized porphyrins, photocurrents are low because of low injection yields and slow electron self-exchange between oxidized porphyrins. As a result, the free-base porphyrins are stable under conditions of water photoelectrolysis and in some cases photovoltages in excess of 1 V are observed.},
doi = {10.1073/pnas.1414901112},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 6,
volume = 112,
place = {United States},
year = {Mon Jan 12 00:00:00 EST 2015},
month = {Mon Jan 12 00:00:00 EST 2015}
}
https://doi.org/10.1073/pnas.1414901112
Web of Science
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