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DOE OSTI · 2587795

Fluorine-free strongly dipolar polymers exhibit tunable ferroelectricity

Huang, Jiahao [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000193265320)·Rui, Guanchun [Case Western Reserve Univ., Cleveland, OH (United States); Pennsylvania State Univ., University Park, PA (United States); Arkema, King of Prussia, PA (United States)] (ORCID:0000000240972205)·Yan, Yueming [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000221580177)·Allahyarov, Elshad [Heinrich-Heine Univ., Dusseldorf (Germany); Russian Academy of Sciences (RAS), Moscow (Russian Federation); Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000172124713)·Kwok, Man-Hin [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000299382648)·Zhu, Wenyi [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000323563159)·Li, Li [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000260889214)·Zhang, Shixian [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000324104560)·Pan, Zhiliang [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000261542765)·Li, Deyu [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000183640924)·Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825)·Mu, Richard R. [Tennessee State Univ., Nashville, TN (United States)] (ORCID:0000000282865934)·Zhao, Bin [Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0000000155059390)·Wang, Qing [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000259683235)·Taylor, Philip L. [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000150602833)·Haglund, Richard F. [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000227011768)·Zhang, Q. M. [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000271500817)·Zhu, Lei [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000165709123)

Abstract

Current research on ferroelectric polymers centers predominantly on poly(vinylidene fluoride) (PVDF)–based fluoropolymers because of their superior performance. However, they are considered “forever chemicals” with environmental concerns. Here, we describe a family of rationally designed fluorine-free ferroelectric polymers, featuring a polyoxypropylene main chain and disulfonyl alkyl side chains with a C3 spacer: −SO 2 CH 2 CHRCH 2 SO 2 − (R = −H or −CH 3 ). Both experimental and simulation results demonstrate that strong dipole-dipole interactions between neighboring disulfonyl groups induce ferroelectric ordering in the condensed state, which can be tailored by changing the R group: ferroelectric for R = −H or relaxor ferroelectric for R = −CH 3 . At low electric fields, the relaxor polymer exhibits electroactuation and electrocaloric performance comparable with those of state-of-the-art PVDF-based tetrapolymers.

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Huang, Jiahao [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000193265320), Rui, Guanchun [Case Western Reserve Univ., Cleveland, OH (United States); Pennsylvania State Univ., University Park, PA (United States); Arkema, King of Prussia, PA (United States)] (ORCID:0000000240972205), Yan, Yueming [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000221580177), Allahyarov, Elshad [Heinrich-Heine Univ., Dusseldorf (Germany); Russian Academy of Sciences (RAS), Moscow (Russian Federation); Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000172124713), Kwok, Man-Hin [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000299382648), Zhu, Wenyi [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000323563159), Li, Li [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000260889214), Zhang, Shixian [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000324104560), Pan, Zhiliang [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000261542765), Li, Deyu [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000183640924), Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825), Mu, Richard R. [Tennessee State Univ., Nashville, TN (United States)] (ORCID:0000000282865934), Zhao, Bin [Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0000000155059390), Wang, Qing [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000259683235), Taylor, Philip L. [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000150602833), Haglund, Richard F. [Vanderbilt Univ., Nashville, TN (United States)] (ORCID:0000000227011768), Zhang, Q. M. [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000271500817), Zhu, Lei [Case Western Reserve Univ., Cleveland, OH (United States)] (ORCID:0000000165709123). 2025-07-03. Fluorine-free strongly dipolar polymers exhibit tunable ferroelectricity. https://doi.org/10.1126/science.ads4702

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