High-entropy polymer produces a giant electrocaloric effect at low fields

More than a decade of research on the electrocaloric (EC) effect has resulted in EC materials and EC multilayer chips that satisfy a minimum EC temperature change of 5 K required for caloric heat pumps(1-3). However, these EC temperature changes are generated through the application of high electric fields(4-8) (close to their dielectric breakdown strengths), which result in rapid degradation and fatigue of EC performance. Here we report a class of EC polymer that exhibits an EC entropy change of 37.5 J kg(-1) K-1 and a temperature change of 7.5 K under 50 MV m(-1), a 275% enhancement over the state-of-the-art EC polymers under the same field strength. We show that converting a small number of the chlorofluoroethylene groups in poly(vinylidene fluoride-trifluoroethylenechlorofluoroethylene) terpolymer into covalent double bonds markedly increases the number of the polar entities and enhances the polar-nonpolar interfacial areas of the polymer. The polar phases in the polymer adopt a loosely correlated, high-entropy state with a low energy barrier for electric-field-induced switching. The polymer maintains performance for more than one million cycles at the low fields necessary for practical EC cooling applications, suggesting that this strategy may yield materials suitable for use in caloric heat pumps.

Automated summary

A new class of EC polymer has been developed, showing significantly enhanced performance under lower electric fields compared to state-of-the-art materials. This improvement is achieved by increasing the number of polar entities in the polymer through the conversion of a small number of chlorofluoroethylene groups into covalent double bonds. The polymer displays high-entropy polar phases with low energy barrier for electric-field-induced switching, maintaining performance for over one million cycles at low fields suitable for practical EC cooling applications.