<p>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 (Bi<sub>1/8</sub>​Na<sub>1/8</sub>​Nd<sub>1/8</sub>​Ag<sub>1/8</sub>​Sr<sub>1/8</sub>​La<sub>1/8</sub>​K<sub>1/8</sub>​Ba<sub>1/8</sub>​)TiO<sub>3</sub> achieved a high recoverable energy storage density of 5.19&#xa0;J/cm<sup>3</sup> and a high energy storage efficiency of 90% under a moderate electric field of 390&#xa0;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&#xa0;MW/cm<sup>3</sup> and an ultrafast discharge time (t<sub>0.9</sub>​) of 27&#xa0;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.</p>

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High energy storage performance of high-entropy lead-free ceramics via A-site co-doping

  • Nianshun Zhao,
  • Juan Hu,
  • Sha Lu,
  • Qin Gao,
  • Liujin Chang,
  • Xinyuan Wang,
  • Shubo Zhang,
  • Shoucheng Tong,
  • Jiale li

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 (Bi1/8​Na1/8​Nd1/8​Ag1/8​Sr1/8​La1/8​K1/8​Ba1/8​)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.