Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation
Abstract
Solution-processable organic semiconductors have potentials as visible photoelectrochemical (PEC) water splitting photoelectrodes due to their tunable small band gap and electronic energy levels, but they are typically limited by poor stability and photocatalytic activity. In this study, we demonstrate the direct visible PEC water oxidation on solution-processed organic semiconductor thin films with improved stability and performance by ultrathin metal oxide passivation layers. N-type fullerene-derivative thin films passivated by sub-2 nm ZnO via atomic layer deposition enabled the visible PEC water oxidation at wavelengths longer than 600 nm in harsh alkaline electrolyte environments with up to 30 μA/cm 2 photocurrents at the thermodynamic water-oxidation equilibrium potential and the photoanode half-lifetime extended to ~1000 s. The systematic investigation reveals the enhanced water oxidation catalytic activity afforded by ZnO passivation and the charge tunneling governing the hole transfer through passivation layers. Further enhanced PEC performances were realized by improving the bottom ohmic contact to the organic semiconductor, achieving ~60 μA/cm 2 water oxidation photocurrent at the equilibrium potential, the highest values reported for organic semiconductor thin films to our knowledge. The improved stability and performance of passivated organic photoelectrodes and discovered design rationales provide useful guidelines for realizing the stable visible solar PECmore »
- Authors:
-
- Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
- Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1430867
- Report Number(s):
- BNL-203414-2018-JAAM
Journal ID: ISSN 0897-4756; TRN: US1802761
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 2; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Atomic layer deposition; solar water splitting; organic semiconductor; ZnO; passivation; photoelectrochemical
Citation Formats
Wang, Lei, Yan, Danhua, Shaffer, David W., Ye, Xinyi, Layne, Bobby H., Concepcion, Javier J., Liu, Mingzhao, and Nam, Chang-Yong. Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b02889.
Wang, Lei, Yan, Danhua, Shaffer, David W., Ye, Xinyi, Layne, Bobby H., Concepcion, Javier J., Liu, Mingzhao, & Nam, Chang-Yong. Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation. United States. https://doi.org/10.1021/acs.chemmater.7b02889
Wang, Lei, Yan, Danhua, Shaffer, David W., Ye, Xinyi, Layne, Bobby H., Concepcion, Javier J., Liu, Mingzhao, and Nam, Chang-Yong. Wed .
"Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation". United States. https://doi.org/10.1021/acs.chemmater.7b02889. https://www.osti.gov/servlets/purl/1430867.
@article{osti_1430867,
title = {Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation},
author = {Wang, Lei and Yan, Danhua and Shaffer, David W. and Ye, Xinyi and Layne, Bobby H. and Concepcion, Javier J. and Liu, Mingzhao and Nam, Chang-Yong},
abstractNote = {Solution-processable organic semiconductors have potentials as visible photoelectrochemical (PEC) water splitting photoelectrodes due to their tunable small band gap and electronic energy levels, but they are typically limited by poor stability and photocatalytic activity. In this study, we demonstrate the direct visible PEC water oxidation on solution-processed organic semiconductor thin films with improved stability and performance by ultrathin metal oxide passivation layers. N-type fullerene-derivative thin films passivated by sub-2 nm ZnO via atomic layer deposition enabled the visible PEC water oxidation at wavelengths longer than 600 nm in harsh alkaline electrolyte environments with up to 30 μA/cm2 photocurrents at the thermodynamic water-oxidation equilibrium potential and the photoanode half-lifetime extended to ~1000 s. The systematic investigation reveals the enhanced water oxidation catalytic activity afforded by ZnO passivation and the charge tunneling governing the hole transfer through passivation layers. Further enhanced PEC performances were realized by improving the bottom ohmic contact to the organic semiconductor, achieving ~60 μA/cm2 water oxidation photocurrent at the equilibrium potential, the highest values reported for organic semiconductor thin films to our knowledge. The improved stability and performance of passivated organic photoelectrodes and discovered design rationales provide useful guidelines for realizing the stable visible solar PEC water splitting based on organic semiconductor thin films.},
doi = {10.1021/acs.chemmater.7b02889},
url = {https://www.osti.gov/biblio/1430867},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 2,
volume = 30,
place = {United States},
year = {2017},
month = {12}
}
Web of Science
Figures / Tables:

Works referencing / citing this record:
Controlled Surface Modification of ZnO Nanostructures with Amorphous TiO 2 for Photoelectrochemical Water Splitting
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- Gasparotto, Alberto; Maccato, Chiara; Sada, Cinzia
- Advanced Sustainable Systems, Vol. 3, Issue 9
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journal, May 2018
- Peng, Guiming; Volokh, Michael; Tzadikov, Jonathan
- Advanced Energy Materials, Vol. 8, Issue 23
Organic Semiconductor Based Devices for Solar Water Splitting
journal, October 2018
- Yao, Liang; Rahmanudin, Aiman; Guijarro, Néstor
- Advanced Energy Materials, Vol. 8, Issue 32
High performance photoanodic catalyst prepared from an active organic photovoltaic cell – high potential gain from visible light
journal, January 2019
- Nagai, Keiji; Kuwabara, Takayuki; Ahmad, Mohd Fairus
- Chemical Communications, Vol. 55, Issue 83
Figures / Tables found in this record: