Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields

A key component of cooling devices is the transfer of entropy from the cold load to heat sink. An electrocaloric (EC) polymer capable of generating both large electrocaloric effect (ECE) and substantial electroactuation can enable EC cooling devices to pump heat without external mechanisms, resultin...

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Main Authors: Guanchun Rui, Wenyi Zhu, Li Li, Jongcheol Lee, Yiwen Guo, Qin Zou, Siyu Wu, Ruipeng Li, Thierry Lannuzel, Fabrice Domingues Dos Santos, Mark A. Aubart, Seong H. Kim, Long‐Qing Chen, Lei Zhu, Zi‐Kui Liu, Q. M. Zhang
Format: Article
Language:English
Published: Wiley-VCH 2025-06-01
Series:Small Science
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Online Access:https://doi.org/10.1002/smsc.202400624
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author Guanchun Rui
Wenyi Zhu
Li Li
Jongcheol Lee
Yiwen Guo
Qin Zou
Siyu Wu
Ruipeng Li
Thierry Lannuzel
Fabrice Domingues Dos Santos
Mark A. Aubart
Seong H. Kim
Long‐Qing Chen
Lei Zhu
Zi‐Kui Liu
Q. M. Zhang
author_facet Guanchun Rui
Wenyi Zhu
Li Li
Jongcheol Lee
Yiwen Guo
Qin Zou
Siyu Wu
Ruipeng Li
Thierry Lannuzel
Fabrice Domingues Dos Santos
Mark A. Aubart
Seong H. Kim
Long‐Qing Chen
Lei Zhu
Zi‐Kui Liu
Q. M. Zhang
author_sort Guanchun Rui
collection DOAJ
description A key component of cooling devices is the transfer of entropy from the cold load to heat sink. An electrocaloric (EC) polymer capable of generating both large electrocaloric effect (ECE) and substantial electroactuation can enable EC cooling devices to pump heat without external mechanisms, resulting in compact designs and enhanced efficiency. However, achieving both high ECE and significant electroactuation remains challenging. Herein, it is demonstrated that poly(vinylidene fluoride‐trifluoroethylene‐chlorofluoroethylene‐double bond) [P(VDF‐TrFE‐CFE‐DB)] tetrapolymers can simultaneously generate high electrocaloric effects and electroactuations under low fields. These P(VDF‐TrFE‐CFE‐DB) tetrapolymers are synthesized through the dehydrochlorination of P(VDF‐TrFE‐CFE) terpolymer. By facile tuning the composition of the initial terpolymer to avoid pure relaxor state, tetrapolymers with optimal DB compositions are achieved, near the critical endpoint of normal ferroelectric phase with diffused phase transition. The nearly vanishing energy barriers between the nonpolar to polar phases result in a strong electrocaloric response and significant electroactuation. Specifically, the P(VDF‐TrFE‐CFE‐DB) tetrapolymer exhibits an EC entropy change ΔS of 100 J kg−1 K−1 under 100 MV m−1: comparable to state‐of‐the‐art (SOA) EC polymers, while delivering nearly twice the electroactuation of the SOA EC polymers. This work presents a general strategy for developing EC materials that combine large electrocaloric effect and electroactuation at low electric fields.
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spelling doaj-art-25df64f4e6af40a0b84a1c63c7b2e9d02025-08-20T02:06:26ZengWiley-VCHSmall Science2688-40462025-06-0156n/an/a10.1002/smsc.202400624Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low FieldsGuanchun Rui0Wenyi Zhu1Li Li2Jongcheol Lee3Yiwen Guo4Qin Zou5Siyu Wu6Ruipeng Li7Thierry Lannuzel8Fabrice Domingues Dos Santos9Mark A. Aubart10Seong H. Kim11Long‐Qing Chen12Lei Zhu13Zi‐Kui Liu14Q. M. Zhang15Arkema Inc. 900 First Avenue King of Prussia PA 19406 USASchool of Electrical Engineering and Computer Science Materials Research Institute The Pennsylvania State University University Park PA 16802 USADepartment of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USADepartment of Chemical Engineering The Pennsylvania State University University Park PA 16802 USADepartment of Chemical Engineering The Pennsylvania State University University Park PA 16802 USADepartment of Macromolecular Science and Engineering Case Western Reserve University Cleveland OH 44106 USANational Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USANational Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USAArkema‐Piezotech Rue Henri‐Moissan 69493 Pierre‐Benite Cedex FranceArkema‐Piezotech Rue Henri‐Moissan 69493 Pierre‐Benite Cedex FranceArkema Inc. 900 First Avenue King of Prussia PA 19406 USADepartment of Chemical Engineering The Pennsylvania State University University Park PA 16802 USADepartment of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USADepartment of Macromolecular Science and Engineering Case Western Reserve University Cleveland OH 44106 USADepartment of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USASchool of Electrical Engineering and Computer Science Materials Research Institute The Pennsylvania State University University Park PA 16802 USAA key component of cooling devices is the transfer of entropy from the cold load to heat sink. An electrocaloric (EC) polymer capable of generating both large electrocaloric effect (ECE) and substantial electroactuation can enable EC cooling devices to pump heat without external mechanisms, resulting in compact designs and enhanced efficiency. However, achieving both high ECE and significant electroactuation remains challenging. Herein, it is demonstrated that poly(vinylidene fluoride‐trifluoroethylene‐chlorofluoroethylene‐double bond) [P(VDF‐TrFE‐CFE‐DB)] tetrapolymers can simultaneously generate high electrocaloric effects and electroactuations under low fields. These P(VDF‐TrFE‐CFE‐DB) tetrapolymers are synthesized through the dehydrochlorination of P(VDF‐TrFE‐CFE) terpolymer. By facile tuning the composition of the initial terpolymer to avoid pure relaxor state, tetrapolymers with optimal DB compositions are achieved, near the critical endpoint of normal ferroelectric phase with diffused phase transition. The nearly vanishing energy barriers between the nonpolar to polar phases result in a strong electrocaloric response and significant electroactuation. Specifically, the P(VDF‐TrFE‐CFE‐DB) tetrapolymer exhibits an EC entropy change ΔS of 100 J kg−1 K−1 under 100 MV m−1: comparable to state‐of‐the‐art (SOA) EC polymers, while delivering nearly twice the electroactuation of the SOA EC polymers. This work presents a general strategy for developing EC materials that combine large electrocaloric effect and electroactuation at low electric fields.https://doi.org/10.1002/smsc.202400624electrocaloricelectrostrictionferroelectric polymers
spellingShingle Guanchun Rui
Wenyi Zhu
Li Li
Jongcheol Lee
Yiwen Guo
Qin Zou
Siyu Wu
Ruipeng Li
Thierry Lannuzel
Fabrice Domingues Dos Santos
Mark A. Aubart
Seong H. Kim
Long‐Qing Chen
Lei Zhu
Zi‐Kui Liu
Q. M. Zhang
Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields
Small Science
electrocaloric
electrostriction
ferroelectric polymers
title Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields
title_full Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields
title_fullStr Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields
title_full_unstemmed Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields
title_short Dual‐Functional High‐Entropy Polymer Exhibiting Giant Cross‐Energy Couplings at Low Fields
title_sort dual functional high entropy polymer exhibiting giant cross energy couplings at low fields
topic electrocaloric
electrostriction
ferroelectric polymers
url https://doi.org/10.1002/smsc.202400624
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