High energy storage performance of high-entropy lead-free ceramics via A-site co-doping
摘要
Driven by the urgent demand for high-performance pulsed power capacitors, a high-entropy strategy was adopted to introduce multiple heterovalent ions into the ceramic matrix for enhancing its configurational entropy. Through the rational screening and combination of various heterovalent ions at the A-site, a strong local random field and chemical disorder were successfully introduced, which disrupted the long-range ferroelectric order and induced the formation of dynamic polar nanoregions. Consequently, a slim P-E hysteresis loop and a high breakdown strength were obtained. As a result, the optimized composition (Bi1/8Na1/8Nd1/8Ag1/8Sr1/8La1/8K1/8Ba1/8)TiO3 achieved a high recoverable energy storage density of 5.19 J/cm3 and a high energy storage efficiency of 90% under a moderate electric field of 390 kV/cm. Benefiting from the enhanced relaxor characteristics and the dense, fine-grained microstructure, the material exhibited outstanding rapid charge–discharge capability and high power intensity, with a power density of 31.5 MW/cm3 and an ultrafast discharge time (t0.9) of 27 ns achieved. Meanwhile, heterovalent doping effectively inhibited defect migration and phase transition, endowing the material with excellent energy storage stability and temperature adaptability over a wide temperature range and a broad frequency range. This work provides an effective material design paradigm for the development of lead-free energy storage dielectrics with high performance and high stability, which are suitable for modern pulsed power systems.