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MATERIALS RESEARCH BULLETIN · 2023 · IF 5.4

Lead-free KNN-based ceramics incorporated with Bi(Zn2/3Nb1/3)O3 possessing excellent optical transmittance and superior energy storage density

Xuewen Peng,Bin Yang,Danjiang Deng,Zhiwei Cai,Xi Kong,Letao Yang,Jinming Guo

The application of lead-free dielectric ceramics for energy storage has received extensive attention because of their remarkable potential as pulse capacitors in power electronic devices. The current study developed a strategy for improving the energy storage performance of (K 0.5 Na 0.5 )NbO 3 (KNN)-based ceramics by incorporating Bi(Zn 2/3 Nb 1/3 )O 3 to reduce grain size, increase dielectric breakdown strength, and enhance ferroelectric relaxation degree. The resulting 0.87KNN–0.13BZN ceramics exhibited a high energy density (7.4 J/cm 3 ) and moderate energy efficiency (74%) at an ultrahigh electric field (750 kV/cm) as well as excellent optical properties. Therefore, the 0.87KNN–0.13BZN ceramic is a promising candidate for pulse capacitors, providing a feasible approach for the development of new lead-free energy storage materials.

研究领域: 材料科学 · 电子工程
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY · 2023 ·Vol. 106 ·期 6 ·3481-3490 · IF 3.9

Crystallographic texture and phase structure induced excellent piezoelectric performance in KNN-based ceramics

Shuo Gao,Peng Li,Jiawei Qu,Wei Li,Jiwei Zhai,Feifei Wang,Jigong Hao,Peng Fu,Zhongbin Pan,Wangfeng Bai

It is difficult to maintain strong piezoelectric properties over a wide temperature range in (K,Na)NbO 3 (KNN)-based ceramics owing to the polymorphic phase boundary (PPB). Here, we propose advantageously utilizing the synergistic effect of crystal orientation and phase structure to address this issue. The 〈0 0 1〉 pc textured (1 − x )(K 0.48 Na 0.52 )(Nb 0.96 Sb 0.04 )O 3 – x (Bi 0.5 Ag 0.5 )ZrO 3 (KNNS– x BAZ) ceramics with different phase structures were synthesized via the templated grain growth method. A high piezoelectric coefficient ( d 33 ) of 505 ± 25 pC/N, an electric field-induced strain of 0.21%, and a superior temperature stability ( d 33 exhibited a high retention of ≥78% at the temperature up to 200°C; strain maintained within 5.7% change over a temperature range of 30–150°C) were simultaneously achieved in textured KNNS–0.03BAZ ceramics. The flattened Gibbs free energy induced by the R–O–T multiphase coexistence, the strong anisotropy of crystals, and the abundant nanodomains contributed to the enhanced piezoelectric properties. The contribution of the strong anisotropy of crystals in 〈0 0 1〉 pc textured ceramics compensates for the deterioration of the piezoelectric properties caused by the phase structure deviation from the PPB with increasing temperature, which benefits the superior temperature stability of the textured KNNS–0.03BAZ ceramics. The previous merits prove that utilizing the synergistic effect of crystal orientation and phase structure is an effective strategy to boost the piezoelectricity and their temperature stability of KNN-based ceramics.

研究领域: 材料科学 · 物理学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Ultrahigh thermal stability and piezoelectricity of lead-free KNN-based texture piezoceramics

Xu Lihui,Lin Jinfeng,Yang Yuxuan,Zhao Zhihao,Shi Xiaoming,Ge Guanglong,Qian Jin,Shi Cheng,Li Guohui,Wang Simin,Zhang Yang,Li Peng,Shen Bo,Fu Zhengqian,Wu Haijun,Huang Houbing,Li Fei,Ding Xiangdong,Sun Jun,Zhai Jiwei

The contradiction between high piezoelectricity and uniquely poor temperature stability generated by polymorphic phase boundary is a huge obstacle to high-performance (K, Na)NbO 3 -based ceramics entering the application market as Pb-based substitutes. We possess the phase boundary by mimicking Pb(Zr, Ti)O 3 ’s morphotropic phase boundary structure via the synergistic optimization of diffusion phase boundary and crystal orientation in 0.94(Na 0.56 K 0.44 )NbO 3 −0.03Bi 0.5 Na 0.5 ZrO 3 −0.03(Bi 0.5 K 0.5 )HfO 3 textured ceramics. As a result, a prominent comprehensive performance is obtained, including giant d 33 of 550 ± 30 pC/N and ultrahigh temperature stability ( d 33 change rate less than 1.2% within 25-150 °C), representing a significant breakthrough in lead-free piezoceramics, even surpassing the Pb-based piezoelectric ceramics. Within the same temperature range, the d 33 change rate of the commercial Pb(Zr, Ti)O 3 −5 ceramics is only about 10%, and more importantly, its d 33 (~ 350 pC/N) is much lower than that of the (K, Na)NbO 3 -based ceramics in this work. This study demonstrates a strategy for constructing the phase boundary with MPB feature, settling the problem of temperature instability in (K, Na)NbO 3 -based ceramics.

研究领域: 材料科学 · 物理学
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2024 · IF 5.8

Significantly enhanced piezoelectric temperature stability of KNN-based ceramics through multilayer textured thick films composite

Peng Li,Shuo Gao,Guangrui Lu,Yang Zhao,Jigong Hao,Peng Fu,Juan Du,Wangfeng Bai,Wei Li,Jiwei Zhai

The temperature instability of piezoelectric properties in KNN-based ceramics has been a major bottleneck impeding them toward practical applications. Herein, we prepared multilayer composite ceramics using two kinds of textured thick films with different polymorphic phase transition temperatures. The composite ceramics simultaneously exhibited outstanding piezoelectric properties (d 33 = 400 ± 20 pC/N; S = 0.18 % at 40 kV/cm) and piezoelectric temperature stability (d 33 and S variation within 5 % and 2 %, respectively over the temperature range of room temperature to 180 °C). The synergistic contribution of slightly fluctuating ε r ·P r values, the robust phase and domain structures, and the complementary effect of piezoelectric fluctuation between the two composite layers led to the outstanding temperature stability of piezoelectric properties . Furthermore, the piezoelectric energy harvester produced using KNN-T 1 /T 2 composite ceramics exhibits a large power density of 5.4 mW/cm 3 . These results prove great potential of KNN-T 1 /T 2 ceramics in high temperature piezoelectric devices.

研究领域: 材料科学 · 物理学
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JOURNAL OF APPLIED PHYSICS · 2024 ·Vol. 136 ·期 7 · IF 2.7

High energy storage performance of KNN-based relaxor ferroelectrics in multiphase-coexisted superparaelectric state

Zha Jielin,Yang Yulong,Liu Jiaxun,Lu Xiaomei,Hu Xueli,Yan Shuo,Wu Zijing,Zhou Min,Huang Fengzhen,Ying Xuenong,Zhu Jinsong

Although K 0.5 Na 0.5 NbO 3 (KNN) possesses large maximum polarization and relatively high breakdown strength, the large remnant polarization constrains their practical applications as energy storage materials. In this work, through multi-element doping, (K 0.5−0.5 x Na 0.5−0.5 x Bi x )(Nb 1− x Sn 0.2 x Zn 0.6 x Ta 0.2 x )O 3 relaxor ferroelectrics were prepared. As the superparaelectric states (SPE) were adjusted to room temperature, orthorhombic, tetragonal, and cubic phases coexisted, accompanied by the highly dynamic polar nanoregions (PNRs). In particular, a high recoverable energy storage density of 4.5 J/cm 3 and an energy storage efficiency of 83% were achieved for the x  = 0.125 ceramic, with the variations less than 11% and 4%, respectively, in the wide temperature range of 20–180 °C. These results demonstrate that the multiphase PNRs in the SPE state is an effective strategy for improving the energy storage performance of KNN-based ceramics.

CAS / MDL: 1314-61-0
研究领域: 材料科学 · 能源存储
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International Journal of Applied Ceramic Technology · 2023 ·Vol. 21 ·期 1 ·493-503 · IF 2.1

High piezoelectric and dielectric constant of Fe/In Co-doped KNN-based ceramics regulated by lattice distortion

Wangzhe Leng,Guoxi Wan,Yanyu Liu,Rui Ma,Yi Du

The new (0.96- x )(K 0.48 Na 0.52 Nb 0.96 Sb 0.04 )O 3 -0.04(Bi 0.5 Ag 0.5 )ZrO 3 - x (Fe 2 O 3 -In 2 O 3 ) ceramics with high dielectric, and electromechanical coupling properties were designed. In this work, the effect of KNN-based ceramics lattice distortion (c/a) and microstructure on the electrical properties was explored by varying the doping amount of Fe 3+ and In 3+ . The problem of a large number of oxygen vacancies generated by the volatilization of K and Na can be well solved by introducing Fe 3+ and In 3+ . The bulk density increases significantly and the maximum value is about 4.52 g/cm 3 .The sample with x = 0.003 has the smallest c/a, and exhibits the best piezoelectric and dielectric properties ( d 33 = 536 pC/N, ε r = 3432 and k p = 55.8 %). Low doping concentration of Fe 2 O 3 is considered a “soft” addition for KNN-based piezoelectric ceramics. The study of this mechanism provides a new idea to regulate the electrical performance of KNN-based ceramics.

研究领域: 材料科学 · 陶瓷工程 · 固体物理
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Optimizing electromechanical properties of KNN-based piezoelectric ceramics through regulation of lattice distortion

Wangzhe Leng,Yanyu Liu,Shu Li,Xinyao Geng,Lu Liu,Yi Du

With the rapid development of broadband transducers, there is an increasing demand for enhanced electromechanical properties in lead-free piezoelectric ceramics. In this study, the strategies to enhance the electrical properties of ceramics were explored by doping BaZrO 3 into 0.96(K 0.48 Na 0.52 )Nb 0.96 Sb 0.04 O 3 -0.04(Bi 0.5 Ag 0.5 )ZrO 3 ceramics, inducing lattice distortion ( c / a ) and regulating the phase structure. The ceramics doped with 1.5 mol% BaZrO 3 demonstrate excellent electrical performance, with a piezoelectric coefficient ( d 33 ) of 545 pC/N, a relative dielectric constant ( ε r ) of 4126, and an electromechanical coupling factor ( k p ) of 54.1 %. The reduced c / a ratio and rhombohedral-orthorhombic-tetragonal phase structure reduce the polarization energy barrier and promote the ordered arrangement of ferroelectric dipoles, thereby enhancing the comprehensive performance of the ceramics. Lastly, the electrical impedance of ceramics is studied in detail and reveals the main conduction mechanism in the microscopic region. This research provides new insights into optimizing the electrical properties of ceramics through microstructural manipulation and demonstrates the potential application of KNN-based ceramics in high performance piezoelectric transducers.

研究领域: 材料科学 · 电陶瓷 · 压电材料
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY · 2022 ·Vol. 106 ·期 5 ·2953-2962 · IF 4.186

KNN-based piezoelectric ceramic multilayer actuators with Ni internal electrodes

Zhihao Dong,Peiyao Zhao,Zhenyong Cen,Xiaohui Wang

On the road of lead-free piezoelectric ceramics into practical applications, the study of Ni-internal-electrode (K, Na)NbO 3 -based (KNN-based) multilayer actuators (MLAs) is an important part, possessing the advantages of environmentally friendly and low cost. The Ni-internal-electrode KNN-based MLAs with different layer numbers and layer thicknesses were fabricated via the tape casting method and sintered in the reducing atmosphere. The piezoelectric layers consist of the main KNN-based phase and a trace amount of second phase Mn 4 Nb 2 O 9 . The element diffusion between the Ni electrodes and KNN-based grains is tiny, indicating that Ni is suitable for co-firing with KNN-based ceramics. After sintering, the compressive stress perpendicular to the thickness direction and the “relative tensile stress” parallel to the thickness direction are retained in the MLAs, bringing influences on the piezoelectric and dielectric properties of KNN-based materials. Compared with the bulk ceramics, the prepared MLAs significantly reduce the driving voltages and increase the displacement outputs, which are more applicable to the scenarios of miniaturization and portability. Particularly, the 46-layer actuator shows high displacements of 1580 and 2737 nm under the voltages of 100 and 200 V, respectively. However, the inverse piezoelectric coefficient d 33 * for each layer of MLAs is still lower than that of the bulk ceramics, indicating that the piezoelectric properties of the KNN-based materials are suppressed. To give full play to the piezoelectric properties of KNN-based materials, more attentions should be paid to the design of reasonable electrode structure and the development of internal electrode paste for MLAs.

研究领域: 材料科学 · 电陶瓷 · 压电材料 · 致动器
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