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Title: Dye-sensitized photoelectrochemical water oxidation through a buried junction

Abstract

Water oxidation has long been a challenge in artificial photosynthetic devices that convert solar energy into fuels. Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) provide a modular approach for integrating light-harvesting molecules with water-oxidation catalysts on metal-oxide electrodes. Despite recent progress in improving the efficiency of these devices by introducing good molecular water-oxidation catalysts, WS-DSPECs have poor stability, owing to the oxidation of molecular components at very positive electrode potentials. Here we demonstrate that a solid-state dye-sensitized solar cell (ss-DSSC) can be used as a buried junction for stable photoelectrochemical water splitting. A thin protecting layer of TiO 2grown by atomic layer deposition (ALD) stabilizes the operation of the photoanode in aqueous solution, although as a solar cell there is a performance loss due to increased series resistance after the coating. With an electrodeposited iridium oxide layer, a photocurrent density of 1.43 mA cm −2was observed in 0.1 M pH 6.7 phosphate solution at 1.23 V versus reversible hydrogen electrode, with good stability over 1 h. We measured an incident photon-to-current efficiency of 22% at 540 nm and a Faradaic efficiency of 43% for oxygen evolution. While the potential profile of the catalyst layer suggested otherwise, we confirmed the formation of amore » buried junction in the as-prepared photoelectrode. The buried junction design of ss-DSSs adds to our understanding of semiconductor–electrocatalyst junction behaviors in the presence of a poor semiconducting material.« less

Authors:
ORCiD logo; ; ; ;
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; China Scholarship Council
OSTI Identifier:
1454669
Alternate Identifier(s):
OSTI ID: 1540295
Grant/Contract Number:  
FG02- 07ER15911; FG02-07ER15911
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: 115 Journal Issue: 27; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; water oxidation; dye-sensitized photoelectrochemical cell; solid-state dye-sensitized solar cell; artificial photosynthesis; dual working electrode

Citation Formats

Xu, Pengtao, Huang, Tian, Huang, Jianbin, Yan, Yun, and Mallouk, Thomas E. Dye-sensitized photoelectrochemical water oxidation through a buried junction. United States: N. p., 2018. Web. doi:10.1073/pnas.1804728115.
Xu, Pengtao, Huang, Tian, Huang, Jianbin, Yan, Yun, & Mallouk, Thomas E. Dye-sensitized photoelectrochemical water oxidation through a buried junction. United States. doi:10.1073/pnas.1804728115.
Xu, Pengtao, Huang, Tian, Huang, Jianbin, Yan, Yun, and Mallouk, Thomas E. Mon . "Dye-sensitized photoelectrochemical water oxidation through a buried junction". United States. doi:10.1073/pnas.1804728115.
@article{osti_1454669,
title = {Dye-sensitized photoelectrochemical water oxidation through a buried junction},
author = {Xu, Pengtao and Huang, Tian and Huang, Jianbin and Yan, Yun and Mallouk, Thomas E.},
abstractNote = {Water oxidation has long been a challenge in artificial photosynthetic devices that convert solar energy into fuels. Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) provide a modular approach for integrating light-harvesting molecules with water-oxidation catalysts on metal-oxide electrodes. Despite recent progress in improving the efficiency of these devices by introducing good molecular water-oxidation catalysts, WS-DSPECs have poor stability, owing to the oxidation of molecular components at very positive electrode potentials. Here we demonstrate that a solid-state dye-sensitized solar cell (ss-DSSC) can be used as a buried junction for stable photoelectrochemical water splitting. A thin protecting layer of TiO2grown by atomic layer deposition (ALD) stabilizes the operation of the photoanode in aqueous solution, although as a solar cell there is a performance loss due to increased series resistance after the coating. With an electrodeposited iridium oxide layer, a photocurrent density of 1.43 mA cm−2was observed in 0.1 M pH 6.7 phosphate solution at 1.23 V versus reversible hydrogen electrode, with good stability over 1 h. We measured an incident photon-to-current efficiency of 22% at 540 nm and a Faradaic efficiency of 43% for oxygen evolution. While the potential profile of the catalyst layer suggested otherwise, we confirmed the formation of a buried junction in the as-prepared photoelectrode. The buried junction design of ss-DSSs adds to our understanding of semiconductor–electrocatalyst junction behaviors in the presence of a poor semiconducting material.},
doi = {10.1073/pnas.1804728115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 27,
volume = 115,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1804728115

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Cited by: 6 works
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