期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 2, 页码 2168-2176出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b19819
关键词
Ag8GeSe6; argyrodites; crystal structure; lattice dynamics; elastic properties; thermoelectric properties
资金
- National Natural Science Foundation of China [51772035, 11604032, 11674040, 51472036, 11874356, 51672270]
- Fundamental Research Funds for the Central Universities [2018 CDQYWL0048, 2018CDPTCG0001/26, 106112017CDJQJ308821, 2018CDJDWL0011, 2018CDYJSY0055]
- CSC scholarship [201806050180]
- Key Research Program of Frontiers Sciences, CAS [QYZDB-SSWSLH016]
- Project for Fundamental and Frontiers Research in Chongqing [CSTC2015JCYJBX0026, CSTC2017jcyjAX0388]
Argyrodites with a general chemical formula of A(8)BX(6) (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 similar to 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.
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