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Combinatorial Synthesis of Oxysulfides in the Lanthanum-Bismuth-Copper System.
ACS Combinatorial Science ( IF 3.903 ) Pub Date : 2020-04-30 , DOI: 10.1021/acscombsci.0c00015
Mitsutaro Umehara 1, 2 , Lan Zhou 1 , Joel A Haber 1 , Dan Guevarra 1 , Kevin Kan 1 , Paul F Newhouse 1 , John M Gregoire 1, 3
Affiliation  

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.

中文翻译:

镧-铋-铜体系的氧硫化物的组合合成。

建立目标材料的合成方法在材料研究中构成了巨大的挑战,这与材料格式的使用启发性规范相结合。使用薄膜材料的太阳能光化学是一种很有前途的技术,正在为此提出许多复杂的材料,本工作描述了组合方法的应用,以探索预测的La–Bi–Cu氧硫化物光电阴极的合成,特别是LaCuOS和BiCuOS的合金。薄膜材料中三种阳离子和两种阴离子的浓度变化及其结晶是通过反应溅射和包括反应退火和快速热处理在内的热过程相结合来实现的。组成和结构表征建立了组成-处理-结构关系,突出了合成LaCuOS和BiCuOS所需的处理条件的广度。La氧化物的相对不可还原性和有限的扩散性表明需要高温处理,这与缓解Bi和S蒸发的温度极限相冲突。总的来说,这些结果表明,这些相的合金将需要专门设计的反应性退火方案以适应每种成分,促进动态处理能力的提高,以进一步自动发现合成路线。
更新日期:2020-04-30
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