High-entropy polymer produces a giant electrocaloric effect at low fields

More than a decade of research on the electrocaloric (EC) effect has resulted in EC materials and EC multilayer chips that satisfy a minimum EC temperature change of 5 K required for caloric heat pumps(1-3). However, these EC temperature changes are generated through the application of high electric fields(4-8) (close to their dielectric breakdown strengths), which result in rapid degradation and fatigue of EC performance. Here we report a class of EC polymer that exhibits an EC entropy change of 37.5 J kg(-1) K-1 and a temperature change of 7.5 K under 50 MV m(-1), a 275% enhancement over the state-of-the-art EC polymers under the same field strength. We show that converting a small number of the chlorofluoroethylene groups in poly(vinylidene fluoride-trifluoroethylenechlorofluoroethylene) terpolymer into covalent double bonds markedly increases the number of the polar entities and enhances the polar-nonpolar interfacial areas of the polymer. The polar phases in the polymer adopt a loosely correlated, high-entropy state with a low energy barrier for electric-field-induced switching. The polymer maintains performance for more than one million cycles at the low fields necessary for practical EC cooling applications, suggesting that this strategy may yield materials suitable for use in caloric heat pumps.

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Work Title High-entropy polymer produces a giant electrocaloric effect at low fields
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Open Access
Creators
  1. Xiaoshi Qian
  2. Donglin Han
  3. Lirong Zheng
  4. Jie Chen
  5. Madhusudan Tyagi
  6. Qiang Li
  7. Feihong Du
  8. Shanyu Zheng
  9. Xingyi Huang
  10. Shihai Zhang
  11. Junye Shi
  12. Houbing Huang
  13. Xiaoming Shi
  14. Jiangping Chen
  15. Hancheng Qin
  16. Jerzy Bernholc
  17. Xin Chen
  18. Long-Qing Chen
  19. Liang Hong
  20. Q. M. Zhang
License In Copyright (Rights Reserved)
Work Type Article
Publisher
  1. Nature
Publication Date December 22, 2021
Publisher Identifier (DOI)
  1. https://doi.org/10.1038/s41586-021-04189-5
Deposited August 11, 2022

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  • Added Creator Sandra Elder
  • Added High-entropy polymer produces a giant electrocaloric effect at low fields.pdf
  • Updated Description, Publication Date, License Show Changes
    Description
    • More than a decade of research on the electrocaloric (EC) effect has resulted in EC materials and EC multilayer chips that satisfy a minimum EC temperature change of 5 K required for caloric heat pumps(1-3). However, these EC temperature changes are generated through the application of high electric fields(4-8) (close to their dielectric breakdown strengths), which result in rapid degradation and fatigue of EC performance. Here we report a class of EC polymer that exhibits an EC entropy change of 37.5 J kg(-1) K-1 and a temperature change of 7.5 K under 50 MV m(-1), a 275% enhancement over the state-of-the-art EC polymers under the same field strength. We show that converting a small number of the chlorofluoroethylene groups in poly(vinylidene fluoride-trifluoroethylenechlorofluoroethylene) terpolymer into covalent double bonds markedly increases the number of the polar entities and enhances the polar-nonpolar interfacial areas of the polymer. The polar phases in the polymer adopt a loosely correlated, high-entropy state with a low energy barrier for electric-field-induced switching. The polymer maintains performance for more than one million cycles at the low fields necessary for practical EC cooling applications, suggesting that this strategy may yield materials suitable for use in caloric heat pumps.
    Publication Date
    • 2022-01-06
    License
    • https://rightsstatements.org/page/InC/1.0/
  • Published
  • Updated Acknowledgments Show Changes
    Acknowledgments
    • Author list: Xiaoshi Qian, Donglin Han, Lirong Zheng, Jie Chen, Madhusudan Tyagi, Qiang Li, Feihong Du, Shanyu Zheng, Xingyi Huang, Shihai Zhang, Junye Shi, Houbing Huang, Xiaoming Shi, Jiangping Chen, Hancheng Qin, Jerzy Bernholc, Xin Chen, Long-Qing Chen, Liang Hong & Q. M. Zhang
  • Updated Publisher, Publisher Identifier (DOI), Publication Date, and 1 more Show Changes
    Publisher
    • Nature
    Publisher Identifier (DOI)
    • https://doi.org/10.1038/s41586-021-04189-5
    Publication Date
    • 2022-01-06
    • 2021-12-22
    Publisher's Statement
    • More than a decade of research on the electrocaloric (EC) effect has resulted in EC materials and EC multilayer chips that satisfy a minimum EC temperature change of 5 K required for caloric heat pumps(1-3). However, these EC temperature changes are generated through the application of high electric fields(4-8) (close to their dielectric breakdown strengths), which result in rapid degradation and fatigue of EC performance. Here we report a class of EC polymer that exhibits an EC entropy change of 37.5 J kg(-1) K-1 and a temperature change of 7.5 K under 50 MV m(-1), a 275% enhancement over the state-of-the-art EC polymers under the same field strength. We show that converting a small number of the chlorofluoroethylene groups in poly(vinylidene fluoride-trifluoroethylenechlorofluoroethylene) terpolymer into covalent double bonds markedly increases the number of the polar entities and enhances the polar-nonpolar interfacial areas of the polymer. The polar phases in the polymer adopt a loosely correlated, high-entropy state with a low energy barrier for electric-field-induced switching. The polymer maintains performance for more than one million cycles at the low fields necessary for practical EC cooling applications, suggesting that this strategy may yield materials suitable for use in caloric heat pumps.
  • Updated Acknowledgments Show Changes
    Acknowledgments
    • Author list: Xiaoshi Qian, Donglin Han, Lirong Zheng, Jie Chen, Madhusudan Tyagi, Qiang Li, Feihong Du, Shanyu Zheng, Xingyi Huang, Shihai Zhang, Junye Shi, Houbing Huang, Xiaoming Shi, Jiangping Chen, Hancheng Qin, Jerzy Bernholc, Xin Chen, Long-Qing Chen, Liang Hong & Q. M. Zhang
  • Deleted Creator Sandra Elder
  • Added Creator Xiaoshi Qian
  • Added Creator Donglin Han
  • Added Creator Lirong Zheng
  • Added Creator Jie Chen
  • Added Creator Madhusudan Tyagi
  • Added Creator Qiang Li
  • Added Creator Feihong Du
  • Added Creator Shanyu Zheng
  • Added Creator Xingyi Huang
  • Added Creator Shihai Zhang
  • Added Creator Junye Shi
  • Added Creator Houbing Huang
  • Added Creator Xiaoming Shi
  • Added Creator Jiangping Chen
  • Added Creator Hancheng Qin
  • Added Creator Jerzy Bernholc
  • Added Creator Xin Chen
  • Added Creator Long-Qing Chen
  • Added Creator Liang Hong
  • Added Creator Q. M. Zhang
  • Updated