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

Wang, Lei; Yan, Danhua; Shaffer, David W.; Ye, Xinyi; Layne, Bobby H.; Concepcion, Javier J.; Liu, Mingzhao; Nam, Chang-Yong

doi:10.1021/acs.chemmater.7b02889

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

Journal Article · Wed Dec 27 00:00:00 EST 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b02889· OSTI ID:1430867

Wang, Lei ^[1]; Yan, Danhua ^[2];

^[3]; Ye, Xinyi ^[1]; Layne, Bobby H. ^[3];

^[3];

^[2];

^[2]

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

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.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1430867

Report Number(s):: BNL-203414-2018-JAAM; TRN: US1802761

Journal Information:: Chemistry of Materials, Vol. 30, Issue 2; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 27 works

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Controlled Surface Modification of ZnO Nanostructures with Amorphous TiO ₂ for Photoelectrochemical Water Splitting Gasparotto, Alberto; Maccato, Chiara; Sada, Cinzia Advanced Sustainable Systems, Vol. 3, Issue 9 https://doi.org/10.1002/adsu.201900046	journal	June 2019

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Related Subjects

14 SOLAR ENERGY
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Atomic layer deposition
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organic semiconductor
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