Superior energy storage performance with a record high breakdown strength in bulk Ba0.85Ca0.15Zr0.1Ti0.9O3-based lead-free ceramics via multiple synergistic strategies

IF 5.3 2区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Nano Materials Pub Date : 2024-10-24 DOI:10.1039/d4qi02126f

Changhao Wang, Jiaxi Hao, Longxiao Duan, Jianfan Zhang, Wenfeng Yue, Zhenhao Fan, Dandan Han, Raz Muhammad, Fanxu Meng, Dawei Wang

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Abstract

A high breakdown strength (E_b) together with a large maximum polarization (P_m) is essential for achieving a high recoverable energy density (W_rec) in energy storage dielectric ceramics. However, meeting the urgent need for practical applications remains a challenge due to the intrinsic properties of bulk dielectric ceramics. Herein, a composition and structure optimization strategy combined with a two-step sintering (TSS) process is proposed to design and fabricate (1−x)Ba_0.85Ca_0.15Zr_0.1Ti_0.9O₃−xBi(Mg_1/2Sn_1/2)O₃ (BCZT-BMSx-TSS) lead-free ceramics. Highly dynamic locally polar nano-regions (PNRs) are formed via composition optimization, exhibiting a very high P_m and energy storage efficiency (η). Compared to the traditional one-step sintering (OSS) process, the TSS process results in a composition with finer grain size and higher density, dramatically increasing E_b. As a result, an ultrahigh energy storage performance with W_rec ∼ 10.53 J cm⁻³ and η ∼ 85.71% is achieved for the BCZT-BMSx-TSS (x = 0.08) ceramic which is attributed to a record high E_b ∼ 830 kV cm⁻¹ and a large P_m ∼ 44.66 μC cm⁻². Complex impedance spectroscopy revealed that the activation energies of the bulk and grain boundary counterparts significantly increased, suggesting an increase in insulation resistance and a decrease in oxygen vacancies, which is the main reason for the high E_b value. In addition, excellent thermal/frequency stability is achieved in both energy density and efficiency, along with good charge–discharge performance. These findings suggest that BCZT-based lead-free ceramics have the potential for practical use in the future.

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通过多种协同策略在块状 Ba0.85Ca0.15Zr0.1Ti0.9O3 无铅陶瓷中实现卓越的储能性能和创纪录的高击穿强度

高击穿强度（Eb）和大最大极化（Pm）是储能电介质陶瓷实现高可回收能量密度（Wrec）的关键。然而，由于块状介电陶瓷的固有特性，要满足实际应用的迫切需求仍是一项挑战。本文提出了一种结合两步烧结 (TSS) 工艺的成分和结构优化策略，用于设计和制造 (1-x)Ba0.85Ca0.15Zr0.1Ti0.9O3-xBi(Mg1/2Sn1/2)O3 (BCZT-BMSx-TSS) 无铅陶瓷。通过成分优化形成了高动态局部极性纳米区域（PNR），表现出极高的 Pm 值和储能效率 (η)。与传统的一步法烧结（OSS）工艺相比，TSS 工艺产生的成分晶粒更细、密度更高，从而显著提高了 Eb。因此，BCZT-BMSx-TSS（x = 0.08）陶瓷实现了 Wrec ∼ 10.53 J cm-3 和 η ∼ 85.71% 的超高储能性能，这归功于创纪录的高 Eb ∼ 830 kV cm-1 和大 Pm ∼ 44.66 μC cm-2。复阻抗光谱显示，块体和晶界对应物的活化能显著增加，表明绝缘电阻增加，氧空位减少，这是 Eb 值高的主要原因。此外，能量密度和效率都实现了出色的热稳定性/频率稳定性，并具有良好的充放电性能。这些研究结果表明，基于 BCZT 的无铅陶瓷在未来具有实际应用的潜力。

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来源期刊

ACS Applied Nano Materials Multiple-

CiteScore

8.30

自引率

3.40%

发文量

1601

期刊介绍： ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.