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Modeling, Simulation, and Fabrication of a Fully Integrated, Acid-stable, Scalable Solar-Driven Water-Splitting System

Walczak, Karl and Chen, Yikai and Karp, Christoph and Beeman, Jeffrey W. and Shaner, Matthew and Spurgeon, Joshua M. and Sharp, Ian D. and Amashukeli, Xenia and West, William and Jin, Jian and Lewis, Nathan S. and Xiang, Chengxiang (2015) Modeling, Simulation, and Fabrication of a Fully Integrated, Acid-stable, Scalable Solar-Driven Water-Splitting System. ChemSusChem, 8 (3). pp. 544-551. ISSN 1864-5631. https://resolver.caltech.edu/CaltechAUTHORS:20150310-113150374

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Abstract

A fully integrated solar-driven water-splitting system comprised of WO3/FTO/p^(+)n Si as the photoanode, Pt/TiO_2/Ti/n^(+)p Si as the photocathode, and Nafion as the membrane separator, was simulated, assembled, operated in 1.0 M HClO_4, and evaluated for performance and safety characteristics under dual side illumination. A multi-physics model that accounted for the performance of the photoabsorbers and electrocatalysts, ion transport in the solution electrolyte, and gaseous product crossover was first used to define the optimal geometric design space for the system. The photoelectrodes and the membrane separators were then interconnected in a louvered design system configuration, for which the light-absorbing area and the solution-transport pathways were simultaneously optimized. The performance of the photocathode and the photoanode were separately evaluated in a traditional three-electrode photoelectrochemical cell configuration. The photocathode and photoanode were then assembled back-to-back in a tandem configuration to provide sufficient photovoltage to sustain solar-driven unassisted water-splitting. The current–voltage characteristics of the photoelectrodes showed that the low photocurrent density of the photoanode limited the overall solar-to-hydrogen (STH) conversion efficiency due to the large band gap of WO_3. A hydrogen-production rate of 0.17 mL hr^−1 and a STH conversion efficiency of 0.24 % was observed in a full cell configuration for >20 h with minimal product crossover in the fully operational, intrinsically safe, solar-driven water-splitting system. The solar-to-hydrogen conversion efficiency, ηS_TH, calculated using the multiphysics numerical simulation was in excellent agreement with the experimental behavior of the system. The value of ηSTH was entirely limited by the performance of the photoelectrochemical assemblies employed in this study. The louvered design provides a robust platform for implementation of various types of photoelectrochemical assemblies, and can provide an approach to significantly higher solar conversion efficiencies as new and improved materials become available.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/cssc.201402896DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/cssc.201402896/abstractPublisherArticle
http://onlinelibrary.wiley.com/doi/10.1002/cssc.201402896/suppinfoPublisherSupporting Information
ORCID:
AuthorORCID
Shaner, Matthew0000-0003-4682-9757
Spurgeon, Joshua M.0000-0002-2987-0865
Sharp, Ian D.0000-0001-5238-7487
Lewis, Nathan S.0000-0001-5245-0538
Xiang, Chengxiang0000-0002-1698-6754
Additional Information:© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. Received: August 26, 2014; Published online on January 7, 2015. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Subject Keywords:multi-physics modeling; prototype; solar fuels; tungsten oxide; water splitting
Issue or Number:3
Record Number:CaltechAUTHORS:20150310-113150374
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150310-113150374
Official Citation:Walczak, K., Chen, Y., Karp, C., Beeman, J. W., Shaner, M., Spurgeon, J., Sharp, I. D., Amashukeli, X., West, W., Jin, J., Lewis, N. S. and Xiang, C. (2015), Modeling, Simulation, and Fabrication of a Fully Integrated, Acid-stable, Scalable Solar-Driven Water-Splitting System. ChemSusChem, 8: 544–551. doi: 10.1002/cssc.201402896
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:55671
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:10 Mar 2015 22:57
Last Modified:09 Mar 2020 13:19

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