Deciphering the structure, dielectric, and energy-storage performances of A-site stoichiometric/nonstoichiometric (Na0.5Bi0.5)TiO3-based ceramics via a two-step optimization design

IF 5.6 2区材料科学 Q1 MATERIALS SCIENCE, CERAMICS Ceramics International Pub Date : 2025-03-01 DOI:10.1016/j.ceramint.2024.12.259

Xiangjun Meng , Ying Yuan , Bin Tang , Enzhu Li

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Abstract

Herein, the stoichiometric ((Na_0.5Bi_0.5)TiO₃ (S_0(N=B)) and (Na_0.36Bi_0.36Sr_0.28)TiO₃ (S_28(N=B))) and nonstoichiometric ((Na_0.3Bi_0.38Sr_0.28)TiO₃ (S_28(N < B)) and (Na_0.42Bi_0.34Sr_0.28)TiO₃ (S_28(N > B))) ceramics were fabricated by a conventional solid-state reaction method. Subsequently, the effects of A-site stoichiometry/nonstoichiometry on their structural, dielectric, and energy-storage performances were investigated. All of them exhibit a single perovskite phase without any impurity phase. S_0(N=B) shows rhombohedral with R3c symmetry, while the other three feature the coexistence of rhombohedral with R3c symmetry and tetragonal with P4bm symmetry. Interestingly, there are significant microstructure and dielectric differences among them. The average grain sizes of S_28(N=B) and S_28(N < B) are smaller than those of S_0(N=B) and S_28(N > B). Notably, S_28(N < B) achieved a significant improvement in dielectric properties. It also exhibited a slim and pinched polarization–electric field hysteresis loop with the largest polarization difference and the smallest electric hysteresis loss, leading to superior energy-storage performance compared to the other three. Subsequently, a tape-casting method (TCM) was employed to prepare S_{28(N < B, TCM)} with improved microstructure and restrained electrical conduction behavior, thereby strengthening the electric breakdown strength from 145 to 200 kV/cm. Consequently, a large recoverable energy density of 2.53 J/cm³ and a high energy conversion efficiency of 83.71 % were realized in S_{28(N < B, TCM)}. Additionally, excellent frequency- and temperature-dependent energy-storage and/or charge-discharge stabilities were confirmed. These results indicate that the structure and electrical properties of (Na_0.5Bi_0.5)TiO₃-based ceramics are sensitive to A-site stoichiometry/nonstoichiometry. They also highlight the superiority of S_{28(N < B, TCM)} over the others, suggesting its promising potential in the dielectric energy-storage field. Furthermore, this work would provide valuable insights into the design and performance optimization of dielectric energy-storage materials/capacitors.

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通过两步优化设计解读a位化学计量/非化学计量（Na0.5Bi0.5） tio3基陶瓷的结构、介电和储能性能

其中，化学计量((Na0.5Bi0.5)TiO3 （S0(N=B)）和（Na0.36Bi0.36Sr0.28）TiO3 （S28(N=B)）和非化学计量((Na0.3Bi0.38Sr0.28)TiO3 (S28(N <；B))和（Na0.42Bi0.34Sr0.28）TiO3 (S28(N >；B)用传统的固相反应方法制备陶瓷。随后，研究了a位化学计量/非化学计量对其结构、介电和储能性能的影响。它们都表现为单一的钙钛矿相，没有任何杂质相。S0（N=B）为R3c对称的菱形体，其他3个为R3c对称的菱形体和P4bm对称的四边形共存。有趣的是，它们之间的微观结构和介电性能存在显著差异。S28（N=B）和S28(N <；B)小于S0（N=B）和S28(N >；值得注意的是，S28(N <；B)在介电性能上取得了显著的改善。其极化差最大，电滞回损耗最小，具有纤细缩窄的极化-电场滞回线，储能性能优于其他三种材料。随后，采用压片法（TCM）制备S28(N <；B， TCM)，改善了微观结构，抑制了导电行为，从而将电击穿强度从145提高到200 kV/cm。结果表明，S28(N <；B,中医)。此外，还证实了优异的频率和温度相关的储能和/或充放电稳定性。这些结果表明，（Na0.5Bi0.5） tio3基陶瓷的结构和电性能对a位化学计量/非化学计量敏感。他们还强调了S28(N <；B， TCM)优于其他，表明其在介电储能领域具有广阔的潜力。此外，这项工作将为介电储能材料/电容器的设计和性能优化提供有价值的见解。

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来源期刊

Ceramics International 工程技术-材料科学：硅酸盐

CiteScore

9.40

自引率

15.40%

发文量

4558

审稿时长

25 days

期刊介绍： Ceramics International covers the science of advanced ceramic materials. The journal encourages contributions that demonstrate how an understanding of the basic chemical and physical phenomena may direct materials design and stimulate ideas for new or improved processing techniques, in order to obtain materials with desired structural features and properties. Ceramics International covers oxide and non-oxide ceramics, functional glasses, glass ceramics, amorphous inorganic non-metallic materials (and their combinations with metal and organic materials), in the form of particulates, dense or porous bodies, thin/thick films and laminated, graded and composite structures. Process related topics such as ceramic-ceramic joints or joining ceramics with dissimilar materials, as well as surface finishing and conditioning are also covered. Besides traditional processing techniques, manufacturing routes of interest include innovative procedures benefiting from externally applied stresses, electromagnetic fields and energetic beams, as well as top-down and self-assembly nanotechnology approaches. In addition, the journal welcomes submissions on bio-inspired and bio-enabled materials designs, experimentally validated multi scale modelling and simulation for materials design, and the use of the most advanced chemical and physical characterization techniques of structure, properties and behaviour. Technologically relevant low-dimensional systems are a particular focus of Ceramics International. These include 0, 1 and 2-D nanomaterials (also covering CNTs, graphene and related materials, and diamond-like carbons), their nanocomposites, as well as nano-hybrids and hierarchical multifunctional nanostructures that might integrate molecular, biological and electronic components.