Abstract

Lead-free bulk ceramics for advanced pulsed power capacitors show relatively low recoverable energy storage density (Wrec) especially at low electric field condition. To address this challenge, we propose an A-site defect engineering to optimize the electric polarization behavior by disrupting the orderly arrangement of A-site ions, in which {rm{B}}{{rm{a}}_{0.105}}{rm{N}}{{rm{a}}_{0.325}}{rm{S}}{{rm{r}}_{0.245 - 1.5x}}{_{0.5x}}{rm{B}}{{rm{i}}_{0.325 + x}}{rm{Ti}}{{rm{O}}_3} ({rm{BN}}{{rm{S}}_{0.245 - 1.5x}}{_{0.5x}}{{rm{B}}_{0.325 + x}}{rm{T}}, x = 0, 0.02, 0.04, 0.06, and 0.08) lead-free ceramics are selected as the representative. The {rm{BN}}{{rm{S}}_{0.245 - 1.5x}}{_{0.5x}}{{rm{B}}_{0.325 + x}}{rm{T}} ceramics are prepared by using pressureless solid-state sintering and achieve large Wrec (1.8 J/cm3) at a low electric field (@110 kV/cm) when x = 0.06. The value of 1.8 J/cm3 is super high as compared to all other Wrec in lead-free bulk ceramics under a relatively low electric field (< 160 kV/cm). Furthermore, a high dielectric constant of 2930 within 15% fluctuation in a wide temperature range of 40–350 °C is also obtained in {rm{BN}}{{rm{S}}_{0.245 - 1.5x}}{_{0.5x}}{{rm{B}}_{0.325 + x}}{rm{T}} (x = 0.06) ceramics. The excellent performances can be attributed to the A-site defect engineering, which can reduce remnant polarization (Pr) and improve the thermal evolution of polar nanoregions (PNRs). This work confirms that the {rm{BN}}{{rm{S}}_{0.245 - 1.5x}}{_{0.5x}}{{rm{B}}_{0.325 + x}}{rm{T}} (x = 0.06) ceramics are desirable for advanced pulsed power capacitors, and will push the development of a series of Bi0.5Na0.5TiO3 (BNT)-based ceramics with high Wrec and high-temperature stability.

Highlights

  • Dielectric capacitor is an indispensable component in contemporary electronic devices, which fulfills different functions such as direct current blocking, coupling, filtering, and pulse discharge [1,2,3]

  • Considering the complicated working environment, especially high temperatures (150–200 °C, even up to 300 °C), ceramic dielectrics would be more suitable for energy storage candidates than other polymer materials [4]

  • Ceramics possess a relatively high Wrec (> 1.5 J/cm3), together with a high (> 70%) under relatively low electric field (< 160 kV/cm), demonstrating that it is potential to obtain both high Wrec and, which should be a promising candidate for power ceramic capacitor application

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Summary

Introduction

Dielectric capacitor is an indispensable component in contemporary electronic devices, which fulfills different functions such as direct current blocking, coupling, filtering, and pulse discharge [1,2,3]. Considering the complicated working environment, especially high temperatures (150–200 °C, even up to 300 °C), ceramic dielectrics would be more suitable for energy storage candidates than other polymer materials [4]. Different methods are utilized to improve Wrec such as chemical doping, glass modification, multilayer structure design, and advanced sintering technology [14,15,16,17,18,19,20,21,22]. Based on our previous work, a binary solid solution of (Bi0.5Na0.5)0.65(Ba0.3Sr0.7)0.35TiO3 (BNT–BST) is considered as a good energy storage material due to “clamped” behavior in P–E loop and high dielectric constant r (~4000) at room temperature [25,26]. The phase structure, micrograph, dielectric temperature stability, and energy storage properties of Ba0.105Na0.325Sr0.245−1.5x 0.5xBi0.325+xTiO3 ceramics are investigated

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