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

Rui, Guanchun; Zhu, Wenyi; Li, Li; Lee, Jongcheol; Guo, Yiwen; Zou, Qin; Wu, Siyu; Li, Ruipeng; Lannuzel, Thierry; Domingues Dos Santos, Fabrice; Aubart, Mark A.; Kim, Seong H.; Chen, Long‐Qing; Zhu, Lei; Liu, Zi‐Kui; Zhang, Q. M.

doi:10.1002/smsc.202400624

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

Journal Article · Sat Feb 22 00:00:00 EST 2025 · Small Science

DOI:https://doi.org/10.1002/smsc.202400624· OSTI ID:2522097

^[1]; ^[2]; Li, Li ^[2]; Lee, Jongcheol ^[2]; Guo, Yiwen ^[2]; Zou, Qin ^[3]; ^[4]; Li, Ruipeng ^[4]; Lannuzel, Thierry ^[5]; Domingues Dos Santos, Fabrice ^[5]; Aubart, Mark A. ^[1]; Kim, Seong H. ^[2]; Chen, Long‐Qing ^[2]; Zhu, Lei ^[3]; Liu, Zi‐Kui ^[2]; ^[2]

Arkema Inc., King of Prussia, PA (United States)
Pennsylvania State Univ., University Park, PA (United States)
Case Western Reserve Univ., Cleveland, OH (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Arkema‐Piezotech (France)

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.

View Journal Article

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2522097

Alternate ID(s):: OSTI ID: 2529402

Report Number(s):: BNL--227668-2025-JAAM

Journal Information:: Small Science, Journal Name: Small Science Journal Issue: 6 Vol. 5; ISSN 2688-4046

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (32)

Enhanced Electrocaloric Response of Vinylidene Fluoride–Based Polymers via One‐Step Molecular Engineering Le Goupil, Florian; Kallitsis, Konstantinos; Tencé‐Girault, Sylvie Advanced Functional Materials, Vol. 31, Issue 1 https://doi.org/10.1002/adfm.202007043	journal	September 2020
Ferroelectric Polymer Nanocomposites for Room-Temperature Electrocaloric Refrigeration Zhang, Guangzu; Li, Qi; Gu, Haiming Advanced Materials, Vol. 27, Issue 8 https://doi.org/10.1002/adma.201404591	journal	January 2015
Challenges and opportunities in piezoelectric polymers: Effect of oriented amorphous fraction in ferroelectric semicrystalline polymers Rui, Guanchun; Allahyarov, Elshad; Zhu, Zhiwen Responsive Materials, Vol. 2, Issue 3 https://doi.org/10.1002/rpm.20240002	journal	May 2024
Electrocaloric Cooling Materials and Devices for Zero-Global-Warming-Potential, High-Efficiency Refrigeration Shi, Junye; Han, Donglin; Li, Zichao Joule, Vol. 3, Issue 5 https://doi.org/10.1016/j.joule.2019.03.021	journal	May 2019
Giant Electrostriction Enabled by Defect-Induced Critical Phenomena in Relaxor Ferroelectric Polymers Chen, Xin; Qin, Hancheng; Zhu, Wenyi Macromolecules, Vol. 56, Issue 2 https://doi.org/10.1021/acs.macromol.2c01952	journal	January 2023
Composition-Dependent Dielectric Properties of Poly(vinylidene fluoride-trifluoroethylene)s Near the Morphotropic Phase Boundary Liu, Yang; Han, Zhubing; Xu, Wenhan Macromolecules, Vol. 52, Issue 17 https://doi.org/10.1021/acs.macromol.9b01403	journal	August 2019
The giant electromechanical response in ferroelectric relaxors as a critical phenomenon Kutnjak, Z.; Petzelt, J.; Blinc, R. Nature, Vol. 441, Issue 7096 https://doi.org/10.1038/nature04854	journal	June 2006
Giant electrocaloric materials energy efficiency in highly ordered lead scandium tantalate Nouchokgwe, Youri; Lheritier, Pierre; Hong, Chang-Hyo Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23354-y	journal	June 2021
A cascade electrocaloric cooling device for large temperature lift Meng, Yuan; Zhang, Ziyang; Wu, Hanxiang Nature Energy, Vol. 5, Issue 12 https://doi.org/10.1038/s41560-020-00715-3	journal	October 2020
The relation of local order to material properties in relaxor ferroelectrics Krogstad, M. J.; Gehring, P. M.; Rosenkranz, S. Nature Materials, Vol. 17, Issue 8 https://doi.org/10.1038/s41563-018-0112-7	journal	June 2018
Large electrocaloric effects in oxide multilayer capacitors over a wide temperature range Nair, B.; Usui, T.; Crossley, S. Nature, Vol. 575, Issue 7783 https://doi.org/10.1038/s41586-019-1634-0	journal	October 2019
High-entropy polymer produces a giant electrocaloric effect at low fields Qian, Xiaoshi; Han, Donglin; Zheng, Lirong Nature, Vol. 600, Issue 7890 https://doi.org/10.1038/s41586-021-04189-5	journal	December 2021
Self-oscillating polymeric refrigerator with high energy efficiency Han, Donglin; Zhang, Yingjing; Huang, Cenling Nature, Vol. 629, Issue 8014 https://doi.org/10.1038/s41586-024-07375-3	journal	May 2024
Hard-to-soft transition-enhanced piezoelectricity in poly(vinylidene fluoride) via relaxor-like secondary crystals activated by high-power ultrasonication Rui, Guanchun; Allahyarov, Elshad; Li, Ruipeng Materials Horizons, Vol. 9, Issue 7 https://doi.org/10.1039/D2MH00442A	journal	January 2022
Influence of composition on relaxor ferroelectric and electromechanical properties of poly(vinylidene fluoride-trifluoroethylene- chlorofluoroethylene) Klein, Rob J.; Xia, Feng; Zhang, Q. M. Journal of Applied Physics, Vol. 97, Issue 9 https://doi.org/10.1063/1.1882769	journal	May 2005
Tunable temperature dependence of electrocaloric effect in ferroelectric relaxor poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene terpolymer Li, Xinyu; Qian, Xiao-shi; Lu, S. G. Applied Physics Letters, Vol. 99, Issue 5 https://doi.org/10.1063/1.3624533	journal	August 2011
Maximizing the number of coexisting phases near invariant critical points for giant electrocaloric and electromechanical responses in ferroelectrics Liu, Z. K.; Li, Xinyu; Zhang, Q. M. Applied Physics Letters, Vol. 101, Issue 8 https://doi.org/10.1063/1.4747275	journal	August 2012
A chip scale electrocaloric effect based cooling device Gu, Haiming; Qian, Xiaoshi; Li, Xinyu Applied Physics Letters, Vol. 102, Issue 12 https://doi.org/10.1063/1.4799283	journal	March 2013
Bulk relaxor ferroelectric ceramics as a working body for an electrocaloric cooling device Plaznik, Uroš; Kitanovski, Andrej; Rožič, Brigita Applied Physics Letters, Vol. 106, Issue 4 https://doi.org/10.1063/1.4907258	journal	January 2015
Coupling of the electrocaloric and electromechanical effects for solid-state refrigeration Bradeško, A.; Juričić, Đ.; Santo Zarnik, M. Applied Physics Letters, Vol. 109, Issue 14 https://doi.org/10.1063/1.4964124	journal	October 2016
Electrocaloric cooling—From materials to devices Chen, Xin; Shvartsman, Vladimir V.; Lupascu, Doru C. Journal of Applied Physics, Vol. 132, Issue 24 https://doi.org/10.1063/5.0132533	journal	December 2022
A self-actuated electrocaloric polymer heat pump design exploiting the synergy of electrocaloric effect and electrostriction Chen, Xin; Zhu, Wenyi; Rattner, Alexander S. Journal of Physics: Energy, Vol. 5, Issue 2 https://doi.org/10.1088/2515-7655/acc278	journal	March 2023
Giant Electrocaloric Effect in Thin-Film PbZr0.95Ti0.05O3 Mischenko, A. S. Science, Vol. 311, Issue 5765 https://doi.org/10.1126/science.1123811	journal	March 2006
Large Electrocaloric Effect in Ferroelectric Polymers Near Room Temperature Neese, B.; Chu, B.; Lu, S.-G. Science, Vol. 321, Issue 5890, p. 821-823 https://doi.org/10.1126/science.1159655	journal	August 2008
Highly efficient electrocaloric cooling with electrostatic actuation Ma, Rujun; Zhang, Ziyang; Tong, Kwing Science, Vol. 357, Issue 6356 https://doi.org/10.1126/science.aan5980	journal	September 2017
A high-performance solid-state electrocaloric cooling system Wang, Yunda; Zhang, Ziyang; Usui, Tomoyasu Science, Vol. 370, Issue 6512 https://doi.org/10.1126/science.aba2648	journal	October 2020
Giant temperature span in electrocaloric regenerator Torelló, A.; Lheritier, P.; Usui, T. Science, Vol. 370, Issue 6512 https://doi.org/10.1126/science.abb8045	journal	October 2020
Relaxor ferroelectric polymer exhibits ultrahigh electromechanical coupling at low electric field Chen, Xin; Qin, Hancheng; Qian, Xiaoshi Science, Vol. 375, Issue 6587 https://doi.org/10.1126/science.abn0936	journal	March 2022
Fluoropolymer ferroelectrics: Multifunctional platform for polar-structured energy conversion Qian, Xiaoshi; Chen, Xin; Zhu, Lei Science, Vol. 380, Issue 6645 https://doi.org/10.1126/science.adg0902	journal	May 2023
High cooling performance in a double-loop electrocaloric heat pump Li, Junning; Torelló, Alvar; Kovacova, Veronika Science, Vol. 382, Issue 6672 https://doi.org/10.1126/science.adi5477	journal	November 2023
Colossal electrocaloric effect in an interface-augmented ferroelectric polymer Zheng, Shanyu; Du, Feihong; Zheng, Lirong Science, Vol. 382, Issue 6674 https://doi.org/10.1126/science.adi7812	journal	December 2023
Self-sustaining personal all-day thermoregulatory clothing using only sunlight Wang, Ziyuan; Bo, Yiwen; Bai, Peijia Science, Vol. 382, Issue 6676 https://doi.org/10.1126/science.adj3654	journal	December 2023

Similar Records

Relaxor ferroelectric polymer exhibits ultrahigh electromechanical coupling at low electric field

Journal Article · Wed Mar 23 20:00:00 EDT 2022 · Science · OSTI ID:1889150

Enhanced piezoelectric response in the artificial ferroelectric polymer multilayers

Journal Article · Sun Nov 30 23:00:00 EST 2014 · Applied Physics Letters · OSTI ID:22402423

Related Subjects

36 MATERIALS SCIENCE
electrocaloric
electrostriction
ferroelectric polymers

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

Citation Formats

References (32)

Similar Records

Related Subjects