Energetics and Solvation Effects at the Photoanode/Catalyst Interface: Ohmic Contact versus Schottky Barrier
Abstract
The design of optimal interfaces between photoelectrodes and catalysts is a key challenge in building photoelectrochemical cells to split water. Iridium,dioxide (IrO2) is an,efficient catalyst for oxygen evolution, stable in acidic conditions, and hence a good candidate, to be. interfaced with photoanodes. Using first-principles quantum mechanical calculations; we investigated the structural and electronic properties of tungsten trioxide (WO3) surfaces interfaced with an IrO2 thin film. We, built a microacopic model of the interface that exhibits a formation energy lower than the surface energy of the most, stable IrO2 surface, in spite of a large lattice Mismatch, and has to impurity states pinning the Fermi.,level. We found that upon full coverage of WO3 by IrO2, the two oxides form undesirable Ohmic contacts. However, our calculatious predicted that if both oxides are partially exposed to water solvent, the relative position of the absorber conduction band and the catalyst Fermi level favors charge transfer to the catalyst and hence water We propose that, for oxide photoelectrodes interfaced with IrO2, it is advantageous to form tough interfaces with the catalyst, e.g., by depositing nanoparticles, instead of sharp interfaces with thin films.
- Authors:
-
- Joint Center for Artificial Photosynthesis, California Institute of Technology and Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Joint Center for Artificial Photosynthesis, California Institute of Technology and Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States
- Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States, Argonne National Laboratory, Lemont, Illinois 60439, United States
- Publication Date:
- Research Org.:
- California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1328817
- Alternate Identifier(s):
- OSTI ID: 1391705
- Grant/Contract Number:
- AC02-06CH11357; SC0004993
- Resource Type:
- Published Article
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Name: Journal of the American Chemical Society Journal Volume: 137 Journal Issue: 16; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalysts; Oxides; Interfaces; Energy; Semiconductors
Citation Formats
Ping, Yuan, Goddard, III, William A., and Galli, Giulia A. Energetics and Solvation Effects at the Photoanode/Catalyst Interface: Ohmic Contact versus Schottky Barrier. United States: N. p., 2015.
Web. doi:10.1021/jacs.5b00798.
Ping, Yuan, Goddard, III, William A., & Galli, Giulia A. Energetics and Solvation Effects at the Photoanode/Catalyst Interface: Ohmic Contact versus Schottky Barrier. United States. https://doi.org/10.1021/jacs.5b00798
Ping, Yuan, Goddard, III, William A., and Galli, Giulia A. Mon .
"Energetics and Solvation Effects at the Photoanode/Catalyst Interface: Ohmic Contact versus Schottky Barrier". United States. https://doi.org/10.1021/jacs.5b00798.
@article{osti_1328817,
title = {Energetics and Solvation Effects at the Photoanode/Catalyst Interface: Ohmic Contact versus Schottky Barrier},
author = {Ping, Yuan and Goddard, III, William A. and Galli, Giulia A.},
abstractNote = {The design of optimal interfaces between photoelectrodes and catalysts is a key challenge in building photoelectrochemical cells to split water. Iridium,dioxide (IrO2) is an,efficient catalyst for oxygen evolution, stable in acidic conditions, and hence a good candidate, to be. interfaced with photoanodes. Using first-principles quantum mechanical calculations; we investigated the structural and electronic properties of tungsten trioxide (WO3) surfaces interfaced with an IrO2 thin film. We, built a microacopic model of the interface that exhibits a formation energy lower than the surface energy of the most, stable IrO2 surface, in spite of a large lattice Mismatch, and has to impurity states pinning the Fermi.,level. We found that upon full coverage of WO3 by IrO2, the two oxides form undesirable Ohmic contacts. However, our calculatious predicted that if both oxides are partially exposed to water solvent, the relative position of the absorber conduction band and the catalyst Fermi level favors charge transfer to the catalyst and hence water We propose that, for oxide photoelectrodes interfaced with IrO2, it is advantageous to form tough interfaces with the catalyst, e.g., by depositing nanoparticles, instead of sharp interfaces with thin films.},
doi = {10.1021/jacs.5b00798},
journal = {Journal of the American Chemical Society},
number = 16,
volume = 137,
place = {United States},
year = {Mon Apr 13 00:00:00 EDT 2015},
month = {Mon Apr 13 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/jacs.5b00798
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