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Lowering thermal conductivity in thermoelectric Ti2−xNiCoSnSb half Heusler high entropy alloys

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Abstract

Ti2−xNiCoSnSb (x = 0.125, 0.250, 0.375, and 0.500) half Heusler (HH) high-entropy thermoelectric alloys were synthesized by the arc melting—ball milling—spark plasma sintering route. The impact of secondary phase content on the thermoelectric properties in these alloys was examined. Ni-rich intermetallic (Ni3Sn2, Ni3Sn4) compounds were observed; the intermetallic content increased for lower Ti content, e.g., Ti1.5NiCoSnSb. A Ni-rich full Heusler (FH) secondary phase was also observed. These results were consistent with first-principles calculations that show that the formation enthalpy of Ti1.5NiCoSnSb was higher than that of Ti2NiCoSnSb and the full Heusler (FH) TiNi2Sn phase. In lower Ti content samples, the electrical conductivity increased, and lattice thermal conductivity decreased at the expense of thermopower owing to higher FH and the Ni3Sn2 phase content. Ti1.5NiCoSnSb exhibited lower lattice thermal conductivity of 3.5 W/mK, compared to 5.4 W/mK at 823 K for Ti2NiCoSnSb due to increased phonon scattering at HH/Ni3Sn2 interfaces. But considering the decreasing power factor with lower Ti content, the maximum ZT obtained in Ti1.875NiCoSnSb (0.171 at 973 K) was only marginally higher than the value for Ti2NiCoSnSb. Further, compositional tuning is hence necessary to maximize the power factor. 

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Data availability

The detailed parameters used for DFT calculations, and the csv files of the raw data are available on request to the corresponding author. Data on densities, EDS analysis, lattice parameters and enthalpies are given in the Supporting data file.

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Acknowledgements

We are thankful to the Department of Metallurgical and Materials Engineering, Indian Institute of Technology Madras for their facilities and technical support that aided the material synthesis and characterization. We are also grateful to the HPCE, IIT Madras for their supercomputing facility (Aqua) that enabled the first-principles studies performed in this study. This work is financially sponsored by AME Programmatic Fund by the Agency for Science, Technology and Research, Singapore under Grant No. A1898b0043 and A18B1b0061.

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Author notes

  1. Soumya Ranjan Mishra and Anirudha Karati have equally contributed to this work.

Authors and Affiliations

  1. Department of Metallurgical and Materials Engineering, Indian Institute of Technology Madras, Chennai, India

    Soumya Ranjan Mishra, Satyesh Kumar Yadav & B. S. Murty

  2. School of Materials Science and Engineering, Nanyang Technological University, Singapore, Singapore

    Soumya Ranjan Mishra, P. S. Sankara Rama Krishnan & R. V. Ramanujan

  3. Department of Chemistry, Indian Institute of Technology Madras, Chennai, India

    Anirudha Karati

  4. International Advanced Research Centre for Powder Metallurgy and New Materials (ARCI), PO Balapur, Hyderabad, India

    Anirudha Karati

  5. Thermoelectric Materials and Devices Laboratory, Department of Physics, Indian Institute of Science, Bangalore, India

    Sanyukta Ghosh & Ramesh Chandra Mallik

  6. CNRS, INRAE, Centrale Lille, UMR 8207 - UMET - Unité Matériaux et Transformations, Univ. Lille, 59000, Lille, France

    Rajashekhara Shabadi

  7. Department of Metallurgical and Materials Engineering, Indian Institute of Technology Hyderabad, Kandi, India

    B. S. Murty

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  1. Soumya Ranjan Mishra
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Contributions

SRM and AK contributed to conceptualization, data curation, formal analysis, investigation, methodology, and writing—original draft. SG contributed to investigation, writing—review and editing. RCM, RS and PSRK contributed to formal analysis and investigation. SKY contributed to formal analysis, writing—review and editing. RVR and BSM contributed to project administration, formal analysis, writing—review, and editing, and supervision.

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Correspondence to B. S. Murty.

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Mishra, S.R., Karati, A., Ghosh, S. et al. Lowering thermal conductivity in thermoelectric Ti2−xNiCoSnSb half Heusler high entropy alloys. J Mater Sci 58, 10736–10752 (2023). https://doi.org/10.1007/s10853-023-08664-4

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