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Tailoring thermoelectric properties of Zr0.43Hf0.57NiSn half-Heusler compound by defect engineering

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Abstract

The thermoelectric transport properties of Zr0.43Hf0.57NiSn half-Heusler compounds were investigated for samples sintered with different spark plasma sintering (SPS) periods: 8, 32 and 72 min. By means of scanning transmission electron microscopy with a high-angular annular dark-field detector (STEM-HAADF), it was found that sintering time affected the defect concentration, namely the amount of Ni interstitial atoms, and created locally ordered inclusions of full-Heusler phase. The structural information, phase composition and electrical transport properties could be consistently explained by the assumption that Ni interstitials give rise to an impurity band situated about 100 meV below the bottom of the conduction band via a self-doping behavior. The impurity band was found to merge with the conduction band for the sample with intermediate SPS time. The effect was ascribed to the gradual dissolution of full-Heusler phase inclusions and production of interstitial Ni defects, which eventually vanished for the sample with the longest sintering time. It was demonstrated that the modification of the density of states near the edge of the conduction band and enhanced overall charge carrier concentration provided by defect engineering led to overall 26% increase in the thermoelectric figure of merit (ZT) with respect to the other samples.

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Acknowledgments

This work was financially supported by German Research Foundation Priority Programme 1386 (No.WE 2803/2-2) and the European Union under Marie Skłodowska-Curie Program (W. J. X.). We also gratefully acknowledge the Laboratorio de Microscopias Avanzadas at Instituto de Nanociencia de Aragon, Universidad de Zaragoza, where the aberration-corrected TEM studies were conducted, and thank Prof. Jürg Hulliger for their critical discussion and comments.

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Authors and Affiliations

  1. Institute of Plasma Physics and Laser Microfusion, Warsaw, 01-497, Poland

    Krzysztof Gałązka

  2. Department of Materials Science, Technische Universität Darmstadt, Darmstadt, 64287, Germany

    Wenjie Xie & Anke Weidenkaff

  3. Laboratory for Solid State Chemistry and Catalysis, Empa, Dübendorf, 8600, Switzerland

    Sascha Populoh & Gesine Büttner

  4. Instituto de Nanociencia de Aragón, Universidad de Zaragoza, Saragossa, 50018, Spain

    Myriam H. Aguirre

  5. Departamento de Física de la Materia Condensada, Universidad de Zaragoza, Saragossa, 50009, Spain

    Myriam H. Aguirre

  6. Laboratorio de Microscopías Avanzadas, Universidad de Zaragoza, Saragossa, 50018, Spain

    Myriam H. Aguirre

  7. Fraunhofer Research Institution for Materials Recycling and Resource Strategies IWKS, Hanau, 63457, Germany

    Songhak Yoon & Anke Weidenkaff

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  1. Krzysztof Gałązka
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Correspondence to Wenjie Xie or Anke Weidenkaff.

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Gałązka, K., Xie, W., Populoh, S. et al. Tailoring thermoelectric properties of Zr0.43Hf0.57NiSn half-Heusler compound by defect engineering. Rare Met. 39, 659–670 (2020). https://doi.org/10.1007/s12598-020-01392-7

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  • DOI: https://doi.org/10.1007/s12598-020-01392-7

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