Authors: Youhao Xiong, Zilong Xie, Sen Xue, Chuanlin Wu, Pengshu Xie, Qin Zhang, Qiang Fu
Published: 2025-06-02
Source: Full article
AbstractFerroelectric polymer‐based electrocaloric (EC) materials are promising for next‐generation solid‐state refrigeration due to their high entropy change, eco‐friendliness, lightweight, and flexibility. The practical application of ferroelectric polymer is significantly constrained by its limited EC performance. The prevalent strategy of incorporating ceramic fillers to enhance EC performance contradicts the requirement for high electric breakdown strength (Eb). In this study, a novel approach is utilized that incorporates hydroxy‐containing organic molecules as sacrificial templates to induce polar entities at the interfaces and create nanopores after evaporation. Based on that, nanopores interface engineering is proposed by systematically elucidating the influence of organic molecular structure and dimensions on nanopore size and interfacial polar phase and revealing an approach for precisely regulating nanopore dimensions and interfacial polar phase. The optimal sample achieve a remarkable entropy change (ΔS) of 94.51 J·kg−1·K−1 and temperature change (ΔT) of 18.47 K at 150 MV m−1 with 124% enhancement, facilitated by weakened correlation of polar phases and massive existence of microcrystals. Since nanopores do not act as macroscopic defects that significantly expedite the breakdown phase's growth, a high Eb of 365 MV m−1 is preserved. This work provides a viable strategy for developing eco‐friendly, high‐performance, and safe EC materials.