Li Zehao, Zheng Yisen, Zhang Yi, Tian Ao, Xie Aiwen, Jiang Xuewen, Xie Xinchun, Gao Xin, Er Xiaokuo, Liu Liqiang, Zuo Ruzhong
Center for Advanced Ceramics, School of Materials Science and Engineering, Anhui Polytechnic University, Wuhu 241000, P.R. China.
Anhui Key Laboratory of Low Temperature Co-fired Materials, School of Chemistry and Materials Engineering, Huainan Normal University, Huainan 232038, P. R. China.
ACS Appl Mater Interfaces. 2025 Jul 16;17(28):40690-40698. doi: 10.1021/acsami.5c06895. Epub 2025 Jul 2.
The development of lead-free dielectric ceramics with superior energy-storage performance is critical for next-generation pulsed-power capacitors. This work presents a breakthrough in lead-free (0.8-)(BiNa)TiO-0.2NaNbO-Bi(MgZr)O relaxor antiferroelectric ceramics featuring temperature-insensitive antipolar nanoregions with 4 symmetry, as confirmed by ex- and in situ XRD, Raman spectroscopy, and TEM analysis. In-situ piezoresponse force microscopy demonstrates the electric-field-driven reversible transformation between the antipolar nanoregions and ferroelectric microdomains, accompanied by rapid recovery kinetics upon field removal. This behavior enables a linear-like polarization-field response with minimal hysteresis. Moreover, the synergistically improved grain morphology and band structure contribute to a significantly enhanced breakdown strength. As a result, a superb recoverable energy density ≈ 8.6 J/cm and a high energy efficiency η ≈ 85.5% are simultaneously achieved under 55 kV/mm in the = 0.20 composition, which also exhibit a remarkable thermal stability ( = 4.2 ± 1.7% J/cm, η = 84.9 ± 4.0%, 20-260 °C) and ultrafast charge-discharge capabilities (Powder density = 264.7 MW/cm, discharge energy density = 5.1 J/cm, discharge time < 30 ns). These findings demonstrate a promising strategy for exploiting lead-free dielectrics with desirable overall energy-storage features for capacitor applications.
开发具有卓越储能性能的无铅介电陶瓷对于下一代脉冲功率电容器至关重要。这项工作在无铅(0.8 -)(BiNa)TiO - 0.2NaNbO - Bi(MgZr)O弛豫反铁电陶瓷方面取得了突破，其具有对温度不敏感的具有4重对称性的反极纳米区域，这已通过原位和非原位XRD、拉曼光谱以及TEM分析得到证实。原位压电力显微镜表明，反极纳米区域和铁电微区之间存在电场驱动的可逆转变，场去除后伴随着快速的恢复动力学。这种行为使得极化 - 场响应呈线性，滞后极小。此外，协同改善的晶粒形态和能带结构有助于显著提高击穿强度。结果，在 = 0.20的成分中，在55 kV/mm下同时实现了出色的可恢复能量密度≈8.6 J/cm³和高能量效率η≈85.5%，其还表现出显著的热稳定性( = 4.2 ± 1.7% J/cm³，η = 84.9 ± 4.0%，20 - 260 °C)和超快充放电能力(功率密度 = 264.7 MW/cm³，放电能量密度 = 5.1 J/cm³，放电时间 < 30 ns)。这些发现展示了一种有前景的策略，用于开发具有理想整体储能特性的无铅电介质以用于电容器应用。
