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High-Entropy Perovskites: An Emergent Class of Oxide Thermoelectrics with Ultralow Thermal Conductivity

  • Ritwik Banerjee
    Ritwik Banerjee
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
  • Sabitabrata Chatterjee
    Sabitabrata Chatterjee
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
    Department of Ceramic Engineering, Indian Institute of Technology (BHU) Varanasi, Varanasi, Uttar Pradesh 221005, India
  • Mani Ranjan
    Mani Ranjan
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
    More by Mani Ranjan
  • Tathagata Bhattacharya
    Tathagata Bhattacharya
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
  • Soham Mukherjee
    Soham Mukherjee
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
    Department of Ceramic Engineering, Indian Institute of Technology (BHU) Varanasi, Varanasi, Uttar Pradesh 221005, India
  • Subhra Sourav Jana
    Subhra Sourav Jana
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
  • Akansha Dwivedi
    Akansha Dwivedi
    Department of Ceramic Engineering, Indian Institute of Technology (BHU) Varanasi, Varanasi, Uttar Pradesh 221005, India
  • , and 
  • Tanmoy Maiti*
    Tanmoy Maiti
    Plasmonics and Perovskites Laboratory, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India
    *Email: [email protected]
    More by Tanmoy Maiti
Cite this: ACS Sustainable Chem. Eng. 2020, 8, 46, 17022–17032
Publication Date (Web):November 5, 2020
https://doi.org/10.1021/acssuschemeng.0c03849
Copyright © 2020 American Chemical Society
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Abstract

Although SrTiO3-based perovskites showed a lot of promise as n-type thermoelectric (TE) materials, they demonstrated a low figure of merit value primarily because of their high lattice thermal conductivity (kl). Researchers found it difficult to reduce kl, as a popular route like nanostructuring did not work well with these perovskites possessing low phonon mean free paths. Here, we put forward a novel strategy of designing high-entropy perovskite (HEP) oxides having five transition metals in the B site to induce more anharmonicity causing enhanced multiphonon scattering in order to decrease kl. Using detailed thermodynamic calculations, we designed and synthesized a highly dense Sr(Ti0.2Fe0.2Mo0.2Nb0.2Cr0.2)O3 HEP ceramic. An ultralow thermal conductivity of 0.7 W/mK at 1100 K was achieved in this n-type rare-earth-free HEP oxide TE material. The concept of designing HEPs to achieve ultralow thermal conductivity potentially opens up a new avenue for enhancing TE performance of environmentally benign bulk oxides for high-temperature TE power generation.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.0c03849.

  • Calculation of Lorenz number, lattice thermal conductivity (κl), and electrical thermal conductivity (κe); the temperature-dependent plots of specific heat, thermal diffusivity, and electronic thermal conductivity; XRF analysis; calculation of the Debye temperature taking into consideration of bulk modulus, sheer modulus, and Poisson’s ratio; and thermodynamic calculation: the mixing enthalpy and entropy part of our HEP material (PDF)

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This article is cited by 9 publications.

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