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DOE OSTI · 3029878

Hierarchal structures tuned electrocaloric and electromechanical performance in PVDF-based tetrapolymers

Rui, Guanchun [Arkema Inc., King of Prussia, PA (United States)]·Zhu, Wenyi [Pennsylvania State Univ., University Park, PA (United States)]·Zou, Qin [Case Western Reserve Univ., Cleveland, OH (United States)]·Li, Li [Pennsylvania State Univ., University Park, PA (United States)]·Wu, Siyu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Li, Ruipeng [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000181763138)·Khayat, Raymond [Arkema Piezotech S.A.S., Pierre-Benite (France). Pierre-Bénite Research Center (CRRA)]·Aubart, Mark A. [Arkema Inc., King of Prussia, PA (United States)]·Lannuzel, Thierry [Arkema Piezotech S.A.S., Pierre-Benite (France). Pierre-Bénite Research Center (CRRA)]·Dos Santos, Fabrice Domingues [Arkema Piezotech S.A.S., Pierre-Benite (France). Pierre-Bénite Research Center (CRRA)]·Zhu, Lei [Case Western Reserve Univ., Cleveland, OH (United States)]·Zhang, Q. M. [Pennsylvania State Univ., University Park, PA (United States)]
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Abstract

Ferroelectrics with multifunctionalities are gaining increased interest in self-actuated electrocaloric effect (ECE) refrigerators. However, achieving high ECE and electromechanical (EM) coupling concomitantly for maximum heat transfer remains challenging. Here we present the structure-property relationship for poly(vinylidene fluoride-co-trifluoroethylene-co-chlorofluoroethylene-co-double bond), P(VDF-TrFE-CFE-DB), tetrapolymer, which exhibited a high ECE entropy change of 66.5 J Kg −1 K −1 and EM strain of −6.1%. We show that thermal treatment can be a key factor influencing multifunctional properties. High-temperature annealing incorporates DB and CFE units into crystalline grains to form extended-chain crystals, enabling CFE units to induce relaxor behavior and DB units to induce large structural changes at low electric fields. This synergy leads to an enhancement in both ECE and EM performances. Furthermore, at an optimized temperature of 50 °C, the annealed films exhibit giant cross-energy coupling, achieving ECE and EM performances of 100.8 J Kg −1 K −1 and −7.6%. This study provides insights into developing new ferroelectric polymers with electroactive multifunctionalities.

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36 MATERIALS SCIENCE

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Rui, Guanchun [Arkema Inc., King of Prussia, PA (United States)], Zhu, Wenyi [Pennsylvania State Univ., University Park, PA (United States)], Zou, Qin [Case Western Reserve Univ., Cleveland, OH (United States)], Li, Li [Pennsylvania State Univ., University Park, PA (United States)], Wu, Siyu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Li, Ruipeng [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000181763138), Khayat, Raymond [Arkema Piezotech S.A.S., Pierre-Benite (France). Pierre-Bénite Research Center (CRRA)], Aubart, Mark A. [Arkema Inc., King of Prussia, PA (United States)], Lannuzel, Thierry [Arkema Piezotech S.A.S., Pierre-Benite (France). Pierre-Bénite Research Center (CRRA)], Dos Santos, Fabrice Domingues [Arkema Piezotech S.A.S., Pierre-Benite (France). Pierre-Bénite Research Center (CRRA)], Zhu, Lei [Case Western Reserve Univ., Cleveland, OH (United States)], Zhang, Q. M. [Pennsylvania State Univ., University Park, PA (United States)]. 2026-02-27. Hierarchal structures tuned electrocaloric and electromechanical performance in PVDF-based tetrapolymers. https://doi.org/10.1038/s41528-026-00553-5

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DOE OSTI2026

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

36 MATERIALS SCIENCE↗