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Title: Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation

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 » water splitting based on organic semiconductor thin films.« less
Authors:
 [1] ;  [2] ; ORCiD logo [3] ;  [1] ;  [3] ; ORCiD logo [3] ; ORCiD logo [2] ; ORCiD logo [2]
  1. Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  2. 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)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Publication Date:
Report Number(s):
BNL-203414-2018-JAAM
Journal ID: ISSN 0897-4756; TRN: US1802761
Grant/Contract Number:
SC0012704
Type:
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)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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
OSTI Identifier:
1430867

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., 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. doi: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. 2017. "Improved Stability and Performance of Visible Photoelectrochemical Water Splitting on Solution-Processed Organic Semiconductor Thin Films by Ultrathin Metal Oxide Passivation". United States. doi: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},
journal = {Chemistry of Materials},
number = 2,
volume = 30,
place = {United States},
year = {2017},
month = {12}
}