Umehara, Mitsutaro and Zhou, Lan and Haber, Joel A. and Guevarra, Dan and Kan, Kevin and Newhouse, Paul F. and Gregoire, John M. (2020) Combinatorial synthesis of oxysulfides in the lanthanum-bismuth-copper system. ACS Combinatorial Science, 22 (6). pp. 319-326. ISSN 2156-8952. doi:10.1021/acscombsci.0c00015. https://resolver.caltech.edu/CaltechAUTHORS:20200430-151239863
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Abstract
Establishing synthesis methods for a target material constitutes a grand challenge in materials research, which is compounded with use-inspired specifications on the format of the material. Solar photochemistry using thin film materials is a promising technology for which many complex materials are being proposed, and the present work describes application of combinatorial methods to explore the synthesis of predicted La–Bi–Cu oxysulfide photocathodes, in particular alloys of LaCuOS and BiCuOS. The variation in concentration of three cations and two anions in thin film materials, and crystallization thereof, is achieved by a combination of reactive sputtering and thermal processes including reactive annealing and rapid thermal processing. Composition and structural characterization establish composition-processing-structure relationships that highlight the breadth of processing conditions required for synthesis of LaCuOS and BiCuOS. The relative irreducibility of La oxides and limited diffusion indicate the need for high temperature processing, which conflicts with the temperature limits for mitigating evaporation of Bi and S. Collectively the results indicate that alloys of these phases will require reactive annealing protocols that are uniquely tailored to each composition, motivating advancement of dynamic processing capabilities to further automate discovery of synthesis routes.
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Additional Information: | © 2020 American Chemical Society. Received: February 5, 2020; Revised: March 10, 2020; Published: April 30, 2020. This study 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 (Award No. DE-SC0004993). Author Contributions: M.U. and L.Z. contributed equally. The authors declare no competing financial interest. | ||||||||||||||
Group: | JCAP | ||||||||||||||
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Subject Keywords: | combinatorial synthesis, oxysulfide, thermal processing, solar fuels | ||||||||||||||
Issue or Number: | 6 | ||||||||||||||
DOI: | 10.1021/acscombsci.0c00015 | ||||||||||||||
Record Number: | CaltechAUTHORS:20200430-151239863 | ||||||||||||||
Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20200430-151239863 | ||||||||||||||
Official Citation: | Combinatorial Synthesis of Oxysulfides in the Lanthanum–Bismuth-Copper System. Mitsutaro Umehara, Lan Zhou, Joel A. Haber, Dan Guevarra, Kevin Kan, Paul F. Newhouse, and John M. Gregoire. ACS Combinatorial Science 2020 22 (6), 319-326; DOI: 10.1021/acscombsci.0c00015 | ||||||||||||||
Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||
ID Code: | 102941 | ||||||||||||||
Collection: | CaltechAUTHORS | ||||||||||||||
Deposited By: | George Porter | ||||||||||||||
Deposited On: | 01 May 2020 14:39 | ||||||||||||||
Last Modified: | 16 Nov 2021 18:16 |
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