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Synthesis, Characterization, and Low Temperature Transport Properties of Eu11–xYbxCd6Sb12 Solid-Solution Zintl Phases

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Department of Chemistry, University of California, One Shields Ave., Davis, California 95616, United States
Department of Physics, University of California, One Shields Ave., Davis, California 95616, United States
Cite this: Inorg. Chem. 2016, 55, 23, 12230–12237
Publication Date (Web):November 14, 2016
https://doi.org/10.1021/acs.inorgchem.6b01947
Copyright © 2016 American Chemical Society

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    Abstract

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    Eu11–xYbxCd6Sb12 Zintl solid solutions have been prepared by tin flux reaction by employing the elements Eu/Yb/Cd/Sb/Sn in the ratio 11 – xp:xp:6:12:30, where xp is an integer less than 11 representing the preparative amount of Eu (11 – xp) and Yb (xp). Efforts to make the Yb compositions for x exceeding ∼3 resulted in structures other than the Sr11Cd6Sb12 structure type. The crystal structures and compositions were determined by single-crystal and powder X-ray diffraction and wavelength-dispersive X-ray analysis measurements. The title solid-solution Zintl compounds crystallize in the centrosymmetric monoclinic space group C2/m (no. 12, Z = 2) as the Sr11Cd6Sb12 structure type (Pearson symbol mC58), and the lattice parameters decrease with increasing ytterbium content. Single crystal X-ray diffraction shows that Yb atoms are not randomly distributed in the Eu sites but have a site preference which can be attributed to size effects. The influence of the rare earth (RE) metal sites on thermal and electronic properties of RE11Cd6Sb12 solid solutions has been studied by measuring their thermoelectric properties from 5 to 300 K after consolidation by either spark plasma sintering (SPS) or hot pressing (HP). Electron microprobe analysis reveals that some of the rare earth metal is lost during SPS; as a result pellets formed through SPS have lower electrical resistivity by an order of magnitude due to increased hole-charge carrier concentrations. While the carrier concentration increases, the mobility decreases due to deficiencies in Eu content. Refinement of powder X-ray diffraction shows that Eu loss is mainly from the Eu1 crystallographic site, which has a unique coordination suggesting that this site plays a key role in the transport properties of RE11Cd6Sb12.

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    CIF of Eu11–xYbxCd6Sb12 (x = 0.4 and 1) solid solutions. (pdf). The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.inorgchem.6b01947.

    • Elemental maps for single crystals and pressed pellets (PDF)

    • CIF of Eu11–xYbxCd6Sb12 (x = 0.4 and 1) solid solutions (CIF)

    • CIF of Eu11–xYbxCd6Sb12 (x = 0.4 and 1) solid solutions (CIF)

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    Cited By

    This article is cited by 7 publications.

    1. Tonghan Yang, Jiliang Zhang, Wei He, Kaimin Shih, Shengshou Ma, Cuiyun He. Tuning structure and magnetic properties of table-like magnetocaloric effect in Er6MnSb2 by zirconium substitution. Journal of Rare Earths 2023, 41 (7) , 1073-1082. https://doi.org/10.1016/j.jre.2022.08.002
    2. Robert Freer, Dursun Ekren, Tanmoy Ghosh, Kanishka Biswas, Pengfei Qiu, Shun Wan, Lidong Chen, Shen Han, Chenguang Fu, Tiejun Zhu, A K M Ashiquzzaman Shawon, Alexandra Zevalkink, Kazuki Imasato, G. Jeffrey Snyder, Melis Ozen, Kivanc Saglik, Umut Aydemir, Raúl Cardoso-Gil, E Svanidze, Ryoji Funahashi, Anthony V Powell, Shriparna Mukherjee, Sahil Tippireddy, Paz Vaqueiro, Franck Gascoin, Theodora Kyratsi, Philipp Sauerschnig, Takao Mori. Key properties of inorganic thermoelectric materials—tables (version 1). Journal of Physics: Energy 2022, 4 (2) , 022002. https://doi.org/10.1088/2515-7655/ac49dc
    3. Susan M. Kauzlarich, Kasey P. Devlin, Christopher J. Perez. Zintl phases for thermoelectric applications. 2021, 157-182. https://doi.org/10.1016/B978-0-12-818535-3.00004-9
    4. Sviatoslav Baranets, Alexander Ovchinnikov, Svilen Bobev. Structural diversity of the Zintl pnictides with rare-earth metals. 2021, 227-324. https://doi.org/10.1016/bs.hpcre.2021.07.001
    5. Alexander Ovchinnikov, Gregory Darone, Bayrammurad Saparov, Svilen Bobev. Exploratory Work in the Quaternary System of Ca–Eu–Cd–Sb: Synthesis, Crystal, and Electronic Structures of New Zintl Solid Solutions. Materials 2018, 11 (11) , 2146. https://doi.org/10.3390/ma11112146
    6. Jing Shuai, Jun Mao, Shaowei Song, Qinyong Zhang, Gang Chen, Zhifeng Ren. Recent progress and future challenges on thermoelectric Zintl materials. Materials Today Physics 2017, 1 , 74-95. https://doi.org/10.1016/j.mtphys.2017.06.003
    7. Alexander Ovchinnikov, Jai Prakash, Svilen Bobev. Crystal chemistry and magnetic properties of the solid solutions Ca 14−x RE x MnBi 11 (RE = La–Nd, Sm, and Gd–Ho; x ≈ 0.6–0.8). Dalton Transactions 2017, 46 (46) , 16041-16049. https://doi.org/10.1039/C7DT03715E

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