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Effects of Codoping with Ga and P on Thermoelectric Properties of Ba8Al16Si30 Clathrate System

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Abstract

We have investigated the effects of Codoping With Ga and P on the thermoelectric properties of the Ba8Al16Si30 clathrate system, attempting to optimize the carrier concentration. The elastic properties, which are important for design of thermoelectric devices, were investigated by ultrasonic testing. Ga/P-codoped specimens with nominal compositions Ba8Al16Ga x Si30−2x P x (x = 1.0, 1.5, 2.0) were prepared by arc melting and spark plasma sintering and their Seebeck coefficient, electrical conductivity, and thermal conductivity were measured. Analytical studies revealed that the total content of Al and Ga, expressed as atoms per formula unit, increased to 15.65 at nominal x = 2.0, exceeding the maximum content (y = 15.16) of Al for the Ba8Al y Si46−y clathrate system. Ultrasonic tests determined the Young’s modulus, shear modulus, bulk modulus, and Poisson’s ratio to be 102.55 GPa, 40.14 GPa, 76.85 GPa, and 0.2775, respectively, for Ba8Al16Ga x Si30−2x P x (x = 2.0). The Hall carrier concentration decreased from ∼1.0 × 1021 cm−3 for Ba8Al y Si46−y to ∼6.3 × 1020 cm−3 for Ba8Al16Ga x Si30−2x P x (x = 2.0), suggesting that Ga/P codoping may be useful for tuning the carrier concentration. The value of the Seebeck coefficient at ∼320 K increased from −46 μV K−1 for Ba8Al y Si46−y to −67 μV K−1 for Ba8Al16Ga x Si30−2x P x (x = 2.0). The dimensionless thermoelectric figure␣of merit ZT at 900 K improved from ∼0.4 for Ba8Al y Si46−y to ∼0.47 for Ba8Al16Ga x Si30−2x P x (x = 2.0).

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Acknowledgements

This study was supported by JSPS KAKENHI Grant No. JP25420763. This paper is based on results obtained from a project commissioned by the New Energy and Industrial Technology Development Organization (NEDO).

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Authors and Affiliations

  1. Department of Electrical Engineering, Tokyo University of Science, Yamaguchi, 1-1-1 Daigaku-dori, Sanyo Onoda, Yamaguchi, 756-0884, Japan

    Hiroaki Anno & Kazuya Okamoto

  2. Graduate School of Engineering, Tokyo University of Science, Yamaguchi, 1-1-1 Daigaku-dori, Sanyo Onoda, Yamaguchi, 756-0884, Japan

    Hiroaki Anno & Takahiro Ueda

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Anno, H., Ueda, T. & Okamoto, K. Effects of Codoping with Ga and P on Thermoelectric Properties of Ba8Al16Si30 Clathrate System. J. Electron. Mater. 46, 1730–1739 (2017). https://doi.org/10.1007/s11664-016-5219-5

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