Broad-Temperature Electrocaloric Effect in Multilayered Ferroelectric Polymer Nanocomposites

While the electrocaloric effect (ECE) presents a promising approach for solid-state thermal management in integrated circuits, the development of ferroelectric materials exhibiting high ECE at elevated temperatures remains a significant bottleneck. Herein, we report multilayered ferroelectric polymer composites that demonstrate a giant ECE across a broad temperature range. By strategically tailoring the electric field distribution and optimizing polarization behavior through the controlled dispersion of ferroelectric ceramic nanofillers in the polymer matrix, as supported by phase-field modeling, the composites show a large adiabatic temperature change (ΔT) of 25.3 K and a high entropy change (ΔS) of 0.25 J cm⁻³ K⁻¹ at room temperature. To further suppress electrical conduction, [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) was introduced into the polymer layers. The multilayered ferroelectric nanocomposites achieve ΔT and ΔS values exceeding 20 K and 0.18 J cm⁻³ K⁻¹, respectively, over a temperature range of 0-80 °C. This work offers a promising design strategy for developing high-performance electrocaloric materials for thermal management in advanced microelectronic systems.