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Broad Distribution of Local Polar States Generates Large Electrothermal Properties in Pb-Free Relaxor Ferroelectrics

  • Frederick P. Marlton
    Frederick P. Marlton
    School of Chemistry, The University of Sydney, Sydney, NSW 2006, Australia
    Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University, 8000 Aarhus C, Denmark
  • Sanjib Nayak
    Sanjib Nayak
    Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China
    More by Sanjib Nayak
  • Sarangi Venkateshwarlu
    Sarangi Venkateshwarlu
    Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China
  • Ngai Hang Chan
    Ngai Hang Chan
    Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China
  • Jing Kong
    Jing Kong
    Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China
    More by Jing Kong
  • Yuanpeng Zhang
    Yuanpeng Zhang
    Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Matthew G. Tucker
    Matthew G. Tucker
    Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Mads Ry Vogel Jørgensen*
    Mads Ry Vogel Jørgensen
    Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University, 8000 Aarhus C, Denmark
    MAX IV Laboratory, Lund University, SE-221 00 Lund, Sweden
    *Email: [email protected] (M.R.V.J.)
  • , and 
  • Abhijit Pramanick*
    Abhijit Pramanick
    Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, China
    *Email: [email protected] (A.P.)
Cite this: Chem. Mater. 2021, 33, 22, 8844–8853
Publication Date (Web):November 5, 2021
https://doi.org/10.1021/acs.chemmater.1c03066
Copyright © 2021 American Chemical Society

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    Abstract

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    Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO3-based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric refrigeration capacity of 115 J/kg. Using local-scale structural analysis, we provide an atomistic model for large electrothermal properties in the newly designed Pb-free ferroelectrics, whereby a temperature-independent continuous distribution of cation displacement directions creates easy pathways for microscopic polarization reorientation. This research provides key structural insight for future atomic-scale engineering of environmentally sustainable ferroelectrics in energy applications.

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    Cited By

    This article is cited by 1 publications.

    1. Jing Kong, Sanjeev K. Nayak, Jue Liu, S. Pamir Alpay, Abhijit Pramanick. Local atomic structure distortions in the Dion-Jacobson ferroelectric CsBi Nb 2 O 7 . Physical Review B 2022, 106 (2) https://doi.org/10.1103/PhysRevB.106.024103