共取代对复杂热电化合物的影响:Zintl 相 Ba1-xSrxZn2-yCuySb2 系统

IF 1.7 4区 化学 Bulletin of the Korean Chemical Society Pub Date : 2023-12-23 DOI:10.1002/bkcs.12806
Jiwon Jeong, Daewon Shim, Myung-Ho Choi, Kang Min Ok, Tae-Soo You
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引用次数: 0

摘要

通过熔融铅金属流法制备了属于 Ba1-xSrxZn2-yCuySb2 (x = 0, 0.09; 0.24 ≤ y ≤ 0.42) 体系的三种共取代四元和二元 Zintl 相。最初使用阳离子 Sr 和阴离子 Cu 对 Ba 和 Zn 进行共取代,以同时降低这些标题化合物的热导率和提高其电导率。通过粉末 X 射线衍射分析验证了单相产物的均匀性,并通过单晶 X 射线衍射分析完善了带有 Ba/Sr 和 Zn/Cu 混合位点的 BaCu2S2 型正方体晶体结构。观察到的 BaCu2S2 型相的结构选择性是通过阳离子元素和阴离子元素的半径比(其中 r+/r- > 1)来合理解释的。利用三种结构模型进行的 DFT 计算表明,Sr 和 Cu 的取代可以提高结构稳定性和空穴载流子浓度。对 BaZn1.76Cu0.24Sb2 和 Ba0.91Sr0.09Zn1.70Cu0.30Sb2 进行的一系列随温度变化的电传输特性测量成功地证明,使用 Sr 和 Cu 共取代可提高导电性,但会降低塞贝克系数,导致功率因数发生轻微变化。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Effect of co-substitution on complex thermoelectric compounds: The Zintl phase Ba1-xSrxZn2-yCuySb2 system

Three co-substituted quaternary and quinary Zintl phases belonging to the Ba1-xSrxZn2-yCuySb2 (x = 0, 0.09; 0.24 ≤ y ≤ 0.42) system were prepared by the molten Pb metal-flux method. Co-substitution using the cationic Sr and anionic Cu for Ba and Zn was initially applied to lower the thermal conductivities and to improve the electric conductivities of these title compounds simultaneously. The homogeneities of single-phase products were verified by powder x-ray diffraction analysis, and the BaCu2S2-type orthorhombic crystal structures with the Ba/Sr and the Zn/Cu mixed-sites were refined by single crystal x-ray diffraction analysis. Structural selectivity for the observed BaCu2S2-type phase was rationalized by the radius ratio of cationic and anionic elements, where r+/r > 1. DFT calculations using the three structural models revealed that the Sr and Cu substitutions can increase the structural stability and the hole carrier concentration. A series of temperature-dependent electrical transport property measurements for BaZn1.76Cu0.24Sb2 and Ba0.91Sr0.09Zn1.70Cu0.30Sb2 successfully proved that the co-substitution using Sr and Cu enhanced electrical conductivities, but reduced the Seebeck coefficients resulting in the slight change in power factor.

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来源期刊
Bulletin of the Korean Chemical Society
Bulletin of the Korean Chemical Society Chemistry-General Chemistry
自引率
23.50%
发文量
182
期刊介绍: The Bulletin of the Korean Chemical Society is an official research journal of the Korean Chemical Society. It was founded in 1980 and reaches out to the chemical community worldwide. It is strictly peer-reviewed and welcomes Accounts, Communications, Articles, and Notes written in English. The scope of the journal covers all major areas of chemistry: analytical chemistry, electrochemistry, industrial chemistry, inorganic chemistry, life-science chemistry, macromolecular chemistry, organic synthesis, non-synthetic organic chemistry, physical chemistry, and materials chemistry.
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