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. 2021 Nov 9;118(45):e2115367118.
doi: 10.1073/pnas.2115367118.

Flexible cyclic-olefin with enhanced dipolar relaxation for harsh condition electrification

Chao Wu  1 , Ajinkya A Deshmukh  2 , Omer Yassin  3 , Jierui Zhou  1   4 , Abdullah Alamri  2 , John Vellek  3 , Stuti Shukla  2 , Michael Sotzing  1 , Riccardo Casalini  5 , Gregory A Sotzing  6   3 , Yang Cao  7   4
Affiliations

Flexible cyclic-olefin with enhanced dipolar relaxation for harsh condition electrification

Chao Wu et al. Proc Natl Acad Sci U S A. .

Abstract

Flexible large bandgap dielectric materials exhibiting ultra-fast charging-discharging rates are key components for electrification under extremely high electric fields. A polyoxafluoronorbornene (m-POFNB) with fused five-membered rings separated by alkenes and flexible single bonds as the backbone, rather than conjugated aromatic structure typically for conventional high-temperature polymers, is designed to achieve simultaneously high thermal stability and large bandgap. In addition, an asymmetrically fluorinated aromatic pendant group extended from the fused bicyclic structure of the backbone imparts m-POFNB with enhanced dipolar relaxation and thus high dielectric constant without sacrificing the bandgap. m-POFNB thereby exhibits an unprecedentedly high discharged energy density of 7.44 J/cm3 and high efficiency at 150 °C. This work points to a strategy to break the paradox of mutually exclusive constraints between bandgap, dielectric constant, and thermal stability in the design of all-organic polymer dielectrics for harsh condition electrifications.

Keywords: dielectric; energy storage; high electric field; polarization; polymer.

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Conflict of interest statement

The authors declare no competing interest.

Figures

Fig. 1.
Fig. 1.
(A) Schematic of the design criteria and mutual constraints for high-temperature high-energy-density energy storage. (B) Chemical structure of m-POFNB. (C) Correlations of m-POFNB with established dielectric polymers in the relationships between bandgap, dielectric constant, and Tg.
Fig. 2.
Fig. 2.
Three-dimensional plot of the (A) dielectric constant and (B) loss as a function of the frequency and temperature.
Fig. 3.
Fig. 3.
Dipole relaxation behavior. (A) The relaxation frequency as a function of the inverse temperature. (B) The density of active dipoles in the relaxation process. (C) The slope of the relaxation peak denoting interactions of dipoles.
Fig. 4.
Fig. 4.
DE loops of m-POFNB at (A) room temperature and (B) 150 °C. (C) Energy storage performance of m-POFNB as a function of the electric field at room temperature and 150 °C. (D) The discharged energy density of m-POFNB relative to the best reported flexible polymers and polymer nanocomposites at 150 °C.
See this image and copyright information in PMC

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