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High-Temperature Structural and Thermoelectric Study of Argyrodite Ag8GeSe6
Shen, Xingchen1,2,3,4; Yang, Chun-Chuen5; Liu, Yamei2; Wang, Guiwen6; Tan, Huan1; Tung, Yung-Hsiang5; Wang, Guoyu3,4; Lu, Xu1; He, Jian2; Zhou, Xiaoyuan1,6
2019
摘要Argyrodites with a general chemical formula of A8BX6 (A = Cu, Ag; B = Si, Ge, Sn; and X = S, Se, and Te) are known for the intimate interplay among mobile ions, electrons, and phonons, which yields rich material physics and materials chemistry phenomena. In particular, the coexistence of fast ionic conduction and promising thermoelectric performance in Ag8GeTe6, Ag8SnSe6, Ag8SiTe6, Ag8SiSe6, and Cu8GeSe6 at high temperatures ushered us to their chemical neighbor Ag8GeSe6, whose high-temperature crystal structure and thermoelectric properties are not yet reported. In this work, we have employed a growth-from-the-melt technique followed by hot pressing to prepare polycrystalline Ag8GeSe6 samples, on which the crystal structure, micro-morphology, compositional analysis, UV-vis absorption, specific heat, speed of sound, and thermoelectric properties were characterized as a function of the Se-deficiency ratio and temperature. We found that (i) the crystal structure of Ag8GeSe6 evolved from orthorhombic at room temperature to face center cubic above 410 K, with a region of phase separations in between; (ii) like other argyrodite 816 phases, Ag8GeSe6 exhibited ultralow thermal conductivities over a wide temperature range as the phonon mean free path was down to the order of interatomic spacing; and (iii) varying Se deficiency effectively optimized the carrier concentration and power factor, a figure of merit zT value ∼0.55 was achieved at 923 K in Ag8GeSe5.88. These results not only fill a knowledge gap of Ag8GeSe6 but also contribute to a comprehensive understanding of 816 phase argyrodites at large. © 2018 American Chemical Society.
DOI10.1021/acsami.8b19819
发表期刊ACS Applied Materials and Interfaces
ISSN19448244
卷号11期号:2页码:2168-2176
收录类别EI
语种英语
EISSN19448252