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Combinatorial synthesis of oxysulfides in the lanthanum-bismuth-copper system

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. 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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acscombsci.0c00015DOIArticle
ORCID:
AuthorORCID
Umehara, Mitsutaro0000-0001-8665-0028
Zhou, Lan0000-0002-7052-266X
Haber, Joel A.0000-0001-7847-5506
Guevarra, Dan0000-0002-9592-3195
Newhouse, Paul F.0000-0003-2032-3010
Gregoire, John M.0000-0002-2863-5265
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
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Subject Keywords:combinatorial synthesis, oxysulfide, thermal processing, solar fuels
Issue or Number:6
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:09 Jun 2020 17:51

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