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Issue 38, 2015
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Structure and properties of type-II clathrate Cs8Na16−xTlxGe136†

Hui Zhang,a   Wei Li,bc   Xuguang Xu,b   Gang Mu,b   Xiaoming Xieb  and  Fuqiang Huang*ad  
Author affiliations

* Corresponding authors

a CAS Key Laboratory of Materials for Energy Conversion and State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. China
E-mail: huangfq@mail.sic.ac.cn

b State Key Laboratory of Functional Materials for Informatics and Shanghai Center for Superconductivity, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, P. R. China

c State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai 200433, P. R. China

d Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China

Abstract

Tl-doped type-II clathrate Cs8Na16−xTlxGe136 was synthesized from its elements. The structure was characterised by single crystal and powder diffraction. Cs8Na16−xTlxGe136 crystallized in the space group Fd[3 with combining macron]m. The melting point decreased with increasing Tl content at 925.0 °C, 922.8 °C and 915.7 °C for Cs8Na14.76(3)Tl1.24(2)Ge136, Cs8Na9.94(2)Tl6.06(2)Ge136 and Cs8Na8.36(2)Tl7.64(2)Ge136 in Ar atmosphere, respectively. Cs8Na9.94(2)Tl6.06(2)Ge136 exhibited diamagnetism with χ = −3.11 × 10−3 emu mol−1 at 1.8 K. The heat capacity of Cs8Na9.94(2)Tl6.06(2)Ge136 presented an Einstein peak at 10 K. The fitted parameters for Cs8Na9.94(2)Tl6.06(2)Ge136 were λ = 0.115(4) J mol−1 K−2, β = 0.0289(2) J mol−1 K−4, NE = 7.94(4), θE = 56.9(1) K, ND = 152.06(4) and θD = 217(1) K using the equation Cp = Ce + CD + CE from 1.8 K to 10 K. The thermoelectric measurement showed metallic resistivity and a negative Seebeck coefficient, indicating electron-type charge carriers. The electronic structure calculation for Cs8Na10Tl6Ge136 confirmed the nature of the metallic transport behavior with conducting electrons, mainly from the Ge p orbitals.

Graphical abstract: Structure and properties of type-II clathrate Cs8Na16−xTlxGe136

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Supplementary files

Article information

https://doi.org/10.1039/C5DT02766G
Submitted
21 Jul 2015
Accepted
24 Aug 2015
First published
27 Aug 2015
Dalton Trans., 2015,44, 16937-16945
Article type
Paper
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Structure and properties of type-II clathrate Cs8Na16−xTlxGe136

H. Zhang, W. Li, X. Xu, G. Mu, X. Xie and F. Huang, Dalton Trans., 2015, 44, 16937
DOI: 10.1039/C5DT02766G

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