Scalable In-situ Microfibrillar dielectric films: Achieving exceptional energy density and efficiency

It is a formidable challenge to develop a feasible strategy for the scalable fabrication of all-organic dielectrics with simultaneous improvements in both discharged energy density (U_d) and efficiency (η). Herein, an innovative technology of “melting extrusion-hot stretching-quenching” was put forward for the large-scale preparation of all-organic polymer dielectric films, where polymethyl methacrylate (PMMA) was miscible with polyvinylidene fluoride (PVDF) to form single dispersed phase in the polypropylene (PP) matrix and in-situ transformed into microfibrils with the aid of elongational flow field. Thereby, a simultaneous enhancement in the dielectric constant and breakdown strength was achieved and the as-prepared PP-based all-polymer dielectric film exhibited an unprecedented ultrahigh U_d of 9.6 J cm⁻³ and an exceptional η of 90.9 %. Experimental verification and computational simulation confirmed that the formation of highly oriented PMMA/PVDF microfibrils and well-aligned interfaces are constructive to enhancing breakdown strength by suppressing electric field distortion. The highly oriented dipoles in PVDF and PMMA, coupled with the eliminated ferroelectric behavior of PVDF, synergistically contributed to the heightened U_d and η. The approach presented in this work opens up a promising avenue for the large-scale production of all-organic capacitor films with enhanced U_d and η, heralding a new era of advanced dielectric materials.