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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Enhanced dielectric relaxation and low-electric-field energy storage properties of NaNbO3 ceramics prepared by co-doping MgO and BiYbO3

Xue Bai,Tao Fan,Gang Chen,Jie Wang,Cong Ji,Chao Chen,Zixuan Zhang,Wei Cai,Rongli Gao,Chunlin Fu

NaMg 0.12 Nb 0.88 O 3 - x BiYbO 3 (abbreviated as NMN- x BY) ( x  = 0, 0.005, 0.01, 0.015, 0.02, 0.04 and 0.08) ceramics were fabricated by using a traditional solid-state reaction method. The crystal structure, morphology, relaxation behavior and energy storage properties of NMN- x BY) ceramics were systematically investigated. X-ray diffraction patterns (XRD) demonstrates that all samples present a single pseudo-cubic phase. It is also found that the grain sizes vary irregular with the BY content, and it can be reduced by the appropriate addition of BY content as indicated by scanning electron morphology. From the measured dielectric properties , it can be seen that all samples are transformed from normal ferroelectric (FEs) to relaxor ferroelectric (RFEs). The maximum relaxor diffuseness coefficient γ (∼1.78) is obtained for 0.98NMN-0.02BY ceramic. As x increases, the polarization-electric ( P - E ) hysteresis loops gradually become slimmer. The largest discharged energy density (∼0.998 J/cm 3 ) and the maximum energy efficiency (∼70%) are obtained at 170 kV/cm for x  = 0.04. Meanwhile, the discharge energy densities present relatively excellent temperature stability for x  = 0.02 in the temperature range from 20 to 140 °C. This work demonstrates a wide potential application in enhancing the storage properties of lead-free ferroelectric materials by co-doping MgO and bismuth-based perovskites .

研究领域: 材料科学 · 电介质物理
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Gels · 2022 ·Vol. 8 ·期 7 ·409 · IF 4.432

Significant Interfacial Dielectric Relaxation of Covalently Bonded Ice-Hydrogels

Yongqiang Li,Liufang Chen,Chuanfu Li,Lin Lin,Zhibo Yan,Junming Liu

Hydrogels are composed of a three-dimensional network of cross-linked hydrophilic polymer chains and large amounts of water. The physicochemical properties of the polymer-water interface in hydrogels draw our attention. Due to the complex structure of hydrogel systems, it is still a challenge to investigate the interfacial layer properties of hydrogels through experiments. In this work, we investigate the properties of the covalently bonded chitosan-based ice-hydrogels interfacial layer by dielectric relaxation spectroscopy (DRS) techniques in the presence of avoided electrode polarization. The DRS data exhibit that the polymer-water interfacial layer has a strong dielectric signal response, which indicates that a large number of polar electric dipoles or polar molecules may be contained in the interfacial layer. The variable temperature dielectric relaxation behavior of a series of chitosan-base ice-hydrogels showed that the value of dielectric activation energy for different water contents is about 180 kJ/mol, which is much larger than that of the polymer and ice phases, suggesting a strong coupling of polar electric dipoles within the interfacial layer. This work demonstrates the important role of the polymer-water interface in covalently bonded hydrogels, which will provide assistance in the design and application of covalently bonded hydrogels.Keywords:chitosan;ice-hydrogels;dielectric relaxation behavior;activation energy;interface

研究领域: 材料科学 · 生物物理学
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Effect of Pr3+ doping on relaxation behavior and strain response of PHT-based piezoelectric ceramics

Yushan Deng,Xi Ouyang,Manwen Yao,Xi Yao

Heterovalent ion doping has influenced the further development of piezoelectric applications. Pr 3+ doping in relaxor ferroelectrics is rarely focused on piezoelectric performance enhancement. 0.51 Pb(Ni 1/3 Nb 2/3 )O 3 -0.49 Pb(Hf 0.3 Ti 0.7 )O 3 (PNN-49PHT) ceramics with Pr 3+ doping ceramics were designed and fabricated by a two-step precursor method. Excellent dielectric diffusion coefficient ( γ ) of 1.96 was achieved at the low Pr 3+ doping concentration of 0.2 %. Increased relaxation enhanced the nanoscale domains formation, resulting in a giant strain response ( d* 33 ) of 1400 pm/V at 10 kV/cm, and a total strain ( S tol ) of 0.27 % at 20 kV/cm. Structural refinement unveiled that the high piezoelectricity originated from the mainly substitution of Pr 3+ for Pb 2+ at the A-site, inducing lattice distortion and phase transitions. Local domain switching and long-range ordered destruction were investigated by piezoresponse force microscopy (PFM) and Scanning Electron Microscopy (SEM). These findings contribute to the advancement of piezoelectric devices and provide valuable insights for the design and optimization of high-performance piezoelectric ceramics .

研究领域: 材料科学 · 物理学
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International Journal of Applied Ceramic Technology · 2023 ·Vol. 21 ·期 1 ·532-543 · IF 2.1

Synergistic modulation of ferroelectric polarization and relaxor behavior of Sr2NaNb5O15-based tungsten bronze ceramic

Peixiaokan Si,Peng Zheng,Xinzhong Zhang,Chong Luo,Xiangting Zheng,Qiaolan Fan,Wangfeng Bai,Jingji Zhang,Liang Zheng,Yang Zhang

Developing dielectric ceramics with high energy storage performance (ESP) is essential for miniaturizing and integrating high-power pulse capacitors. Sr 2 NaNb 5 O 15 -based tungsten bronze ferroelectric ceramics have been highly investigated for dielectric energy storage applications recently. However, the difficulty in concurrently obtaining large polarization and strong relaxor characteristics greatly hinders the ESP improvement. In this work, Bi 3+ and Ti 4+ ions were introduced into the Sr 2 NaNb 5 O 15 ceramic, aiming to modulate the ferroelectric polarization and relaxor behavior synergistically. An excellent recoverable energy density ( W rec ∼ 4.08 J/cm 3 ) and a high efficiency ( η ∼ 84.59%) were concurrently attained in the Sr 1.85 Bi 0.15 NaNb 4.85 Ti 0.15 O 15 composition due to the boosted polarization and enhanced relaxor nature. Moreover, this ceramic also exhibited a high current density (863.06 A/cm 2 ) and a large power density (94.94 MW/cm 3 ). All these characteristics demonstrate that the Bi 3+ and Ti 4+ ions co-doped Sr 2 NaNb 5 O 15 ceramics possess great potential for dielectric capacitor applications.

研究领域: 材料科学 · 无机非金属材料 · 功能陶瓷
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MATERIALS CHEMISTRY AND PHYSICS · 2024 · IF 4.3

Crystalline structure and dielectric relaxor behavior of MnO2-modified 0.8BaTiO3-0.2BiScO3 ceramics for energy storage application

Fujia Ben,Dan Xu,Xinyuan Zhou,Taolin Yu,Jiale Wei,Wenjie Zhao

Based on the synergistic roles of defect dipoles and MnO 2 sintering aid, 0.8BaTiO 3 -0.2BiScO 3 (BTBS 0.2 ) ceramics with and without 0.3 wt% MnO 2 were prepared by a solid-phase reaction route. The impacts of MnO 2 dopant and sintering conditions on the crystalline structure, micro-morphology, dielectric, and energy storage properties were investigated in detail. The X-ray diffraction (XRD) and Raman results demonstrate the coexistence of tetragonal (T) and pseudo-cubic (pC) phases. The increased pC phase content caused by MnO 2 modification is beneficial for the improvement of the relaxation degree. The O 1s fine spectra of X-ray photoelectron spectroscopy (XPS) confirms a remarkable increase in the concentration of oxygen vacancy due to the acceptor Mn dopant, indicating the valence changes of Mn ions from Mn 4+ to Mn 3+ /Mn 2+ . The reduced dielectric loss is induced by the improved density and the pinning effect from the defect dipoles, thereby yielding a higher E b . An optimal energy density of W rec  = 0.70 J/cm 3 with a high energy efficiency of η  = 95.8 % at 140 kV/cm was realized in the BTBS 0.2 +Mn ceramic composition sintered at 1300 °C. Moreover, the ceramic also exhibits good temperature stability (30–120 °C). Therefore, the BTBS 0.2 +Mn ceramics have a promising application prospect in the energy storage field.

研究领域: 材料科学 · 电介质物理
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2024 ·Vol. 35 ·期 26 ·1-13 · IF 2.8

Dielectric properties and impedance spectroscopic study of (1−x)[0.90NaNbO3–0.10Bi(Mg0.5Ta0.5)O3]–x(Bi0.5Na0.5)0.7(Sr0.7La0.2)0.3Ti0.9Zr0.1O3 ceramics

Gao Qin,Zhao Nianshun,Wu Jiale,Yu Qi,Wang Li,Hu Juan,Lu Sha,Zheng Xiaofan

The solid-state reaction method was employed to synthesize (1− x )[0.90NaNbO 3 –0.10Bi(Mg 0.5 Ta 0.5 )O 3 ]– x (Bi 0.5 Na 0.5 ) 0.7 (Sr 0.7 La 0.2 ) 0.3 Ti 0.9 Zr 0.1 O 3 , denoted as (1− x )(NN–BMT)– x BNSLTZ ( x BNSLTZ). XRD analysis of x BNSLTZ confirmed that all samples possessed a pure perovskite structure. SEM micrographs demonstrated homogeneous grain distribution and minimal porosity. With an increasing concentration of BNSLTZ, there was a gradual reduction in average grain size. Impedance spectroscopy was utilized to investigate the electrical properties of x BNSLTZ across a frequency sweep of 10 Hz–1 MHz and over a temperature range of 420–560 °C. The complex impedance and modulus spectra reveal non-Debye-type dielectric relaxation, indicative of two contributing mechanisms: grain and grain boundary effects on conduction. Electric modulus analysis indicated that the low-frequency relaxation process was temperature independent. The dc conductivity variation with temperature follows the Arrhenius equation. The ac conductivity was found to adhere to Jonscher power law. The E a (the relaxation activation energy) and E c (conductance activation energy) confirmed the relaxation mechanism of 0.3BNSLTZ is dipolar conduction. The dielectric properties showed a significant dependence on both frequency and temperature. A dielectric anomaly pointed to the presence of a single relaxation behavior. It was observed that an increase in BNSLTZ concentration led to a decrease in the maximum dielectric constant. Optimum performance was obtained with the 0.3BNSLTZ ceramics, which has the smallest average grain size (1.54 μm), considerable resistance value ( R  ~ 1000 K  \({\Omega }cm\) ), and moderate dielectric constant ( ε r  ~ 600), superior to the pure NN-BMT ceramic. These results demonstrate that the electrical property of the x BNSLTZ ceramics have some potential value in the application of electrical materials.

研究领域: 材料科学 · 物理学
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MATERIALS RESEARCH BULLETIN · 2023 · IF 5.4

Enhanced energy storage performance in Na(Nb,Ta)O3-doped Ba(Ti,Ca)O3-based ceramics through bidirectional optimization strategy

Zhiwei Li,Zhengxiang Bian,Yurong Ren,Zhihui Chen,Jiujun Xu

(1-x)(0.9Ba 1.003 Ti 0.97 Ca 0.03 O 3 –0.1(Bi 0.51 Na 0.47 ) 0.94 Ba 0.06 TiO 3 )-xNa(Nb 0.85 Ta 0.15 )O 3 ( x  = 0.03–0.15) ceramics were designed and fabricated through a bidirectional optimization strategy using traditional solid reaction method. The results revealed that the introduction of Na(Nb 0.85 Ta 0.15 )O 3 increased the vacancy concentration at the A site , conducing to improved polarization and reduced grain size. The substitution at the B site disrupted the long-range ordered ferroelectric domains and generated polar nanodomains, leading to enhanced relaxation behavior. The optimum energy storage density of 3.57 J/cm 3 and efficiency of 87.5% were simultaneously achieved under the electric field of 220 kV/cm in the sample with x  = 0.09. Moreover, it also exhibits extremely high-power density (∼57 MW/cm 3 ), ultrafast discharge time (∼103 ns), high discharge density (1.35 J/cm 3 ), along with excellent temperature (30‒120 °C) and frequency stability (1‒100 Hz) under the equivalent electric field of 120 kV/cm. This novel design strategy provides theoretical guidance for the development of advanced electrical energy storage devices.

研究领域: 材料科学 · 能源存储
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2024 ·Vol. 35 ·期 7 ·1-12 · IF 2.8

Relaxation behavior of BF-BT based ceramics and improved energy storage performance under low electric field

Xie Le-Tian,Zhou Xiao-Xiao,Tang Yu-Cheng,Yin Yang,Hao Yijin,Pei Jun,Zhang Bo-Ping

With the increasing demand for portable electronics, power electronics and other devices, energy storage materials with high power density and large energy storage density are becoming more and more important. BiFeO 3 -BaTiO 3 lead-free ferroelectric ceramics are deemed as a potential lead-free energy storage material due to their high spontaneous polarization and high Curie temperature. However, high remanent polarization has become a serious obstacle to its practical application. In this work, 0.67Bi (1- x ) Sm x FeO 3 -0.33BaTiO 3 (BS x F-BT, 0 ≤  x  ≤ 0.10) was prepared by the conventional solid phase sintering method. The phase transforms from rhombohedral to pseudocubic, and the dielectric and electrical data reveal that relaxor ferroelectrics are favorable for achieving the small size polar nanoregions and enhanced relaxation behavior. Due to enhanced relaxation behavior by doping Sm 3+ , the recoverable energy storage density ( W rec ) reaches 1.99 J/cm 3 , and the energy storage efficiency ( η ) is 57% at a low electric field (190 kV/cm), which is higher than the undoped ceramic ( W rec  = 0.272 J/cm 3 and η  = 26%). This work also puts forward the concept of Ergodic relaxor ferroelectrics and Non-ergodic relaxor ferroelectrics to explain the improvement of energy storage performance.

研究领域: 材料科学 · 物理学
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Journal of Materials Chemistry C · 2022 ·Vol. 10 ·期 43 ·16407-16419 · IF 8.067

Origin of the ultra-wide temperature dielectric stability and dynamic behavior of nanoregions in 0.6Bi(Mg0.5Ti0.5)O3–0.4Ba0.8Ca0.2(Ti0.875Zr0.125)O3

Kaiyuan Chen,Tianxiang Yan,Jia Liu,Xiuyun Lei,Liang Fang,Biaolin Peng,Senentxu Lanceros-Méndez,Dawei Wang,Laijun Liu,Qi Zhang

0.6Bi(Mg0.5Ti0.5)O3–0.4Ba0.8Ca0.2(Ti0.875Zr0.125)O3 (0.6BMT–0.4BCZT) ceramics exhibit an ultrahigh dielectric thermal stability. In this work, the relationship between the local structure and the physical properties of this system is revealed using in situ XRD, in situ Raman, TEM and dielectric responses. It is found that the formation and freezing of both polar nanoregions (PNRs) and nanomosaic structures (NMSs) that comprise ferroelectrically active Ba/Ti rich and weakly polar Bi (and Mg) rich phases are responsible for the high dielectric thermal stability. Three dielectric anomalies, i.e. low-temperature re-entrant dipole-glass-like relaxor behavior, mid-temperature diffuse phase transition (DPT), and high-temperature local phase transitions can be described using the phenomenological statistical model. Furthermore, the relaxor behavior follows the Vogel–Fulcher law and the new glass model. The dipole-glass-like relaxor nature of 0.6BMT–0.4BCZT was characterized by P–E loops. The beta value obtained from the isothermal electrical modulus shows three critical temperatures corresponding to the formations of PNRs, NMS and local phase transition of calcium-containing perovskites.

研究领域: 材料科学 · 物理学
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Preparation and dielectric properties of lead-free perovskite-structured high-entropy ceramics of (La0.25Sr0.25Ba0.25Na0.25)(Ti0.5Me0.5)O3-δ (Me=Sn, Zr, Hf) via doping at both A and B sites

Yingquan Chen,Rui Li,Yan Zhang,Yanping Long,Na Liu,Haijun Xia,Xiong Luo,Bin Meng

A series of lead-free perovskite-structured high-entropy dielectric ceramics with a composition of (La 0.25 Sr 0.25 Ba 0.25 Na 0.25 )(Ti 0.5 Me 0.5 )O 3 (Me = Sn, Zr, Hf) were designed by doping at both the A and B sites. Specifically, these ceramics were prepared via a solid-state reaction method combined with conventional sintering at 1500  ° C for 10 h. All high-entropy ceramics were consisted of a perovskite-structured single solid solution with an average grain size of 2.78–3.85 μm. Of the three samples, (La 0.25 Sr 0.25 Ba 0.25 Na 0.25 )(Ti 0.5 Sn 0.5 )O 3 exhibited the highest dielectric constant, which remained stable from in 25–312  ° C. All three groups of high-entropy ceramics showed typical relaxor behaviour. The discharge energy density ( W d  = 0.31 J/cm 3 ), energy storage efficiency ( η  = 90.88%) and breakdown strength ( BDS  = 300 kV/cm) of (La 0.25 Sr 0.25 Ba 0.25 Na 0.25 )(Ti 0.5 Sn 0.5 )O 3 were much higher than those of BaTiO 3 ( W d  = 0.08 J/cm 3 , η  = 46.09%, BDS  = 30 kV/cm) and other reported lead-free dielectric ceramics. These results demonstrate that high-entropy (La 0.25 Sr 0.25 Ba 0.25 Na 0.25 )(Ti 0.5 Me 0.5 )O 3 ceramics are promising new candidates for high-performance, lead-free dielectric ceramics.

研究领域: 材料科学 · 物理学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

High-temperature relaxation and microwave dielectric response of (1-x)BaNd1.76Bi0.24Ti5O14-xBa0.6Sr0.4La4Ti4O15 compounds with adjustable medium-high dielectric constant

Xiaohui Zhang,Xinyue Zhong,Xiaohua Zhang,Yu Liu,Shuai Ma,Chenglong Yu,Zhenxing Yue

Dielectric ceramics in the microwave band are one of the crucial materials for mobile communication technology, and the studying of their phase evolution and defect behavior can help to understand and reduce dielectric loss. In this work, (1- x )BaNd 1.76 Bi 0.24 Ti 5 O 14 - x Ba 0.6 Sr 0.4 La 4 Ti 4 O 15 ( x = 0.2, 0.4, 0.6 and 0.8, (1- x )BNT- x BSLT) ceramics were synthesized by solid-state reaction method. X-ray diffraction (XRD) and Raman spectra analysis reveal that tungsten bronze and hexagonal perovskite phases coexist in the ceramics, and BaNd 2 Ti 3 O 10 is indexed as the main crystalline phase at x = 0.4, 0.6, leading to a deterioration of the microwave dielectric properties. The defect-related relaxation behavior and its effect on microwave dielectric properties were analyzed by dielectric temperature spectrum and thermally stimulated depolarization current (TSDC). The relationship between the dielectric constant and the electric field distribution was solved using the eigenmode of the high frequency structure simulator. In short, the (1- x )BNT- x BSLT ceramics at x = 0.8 exhibit excellent microwave dielectric properties: ε r = 47.2, Q × f = 16,800 GHz, and τ f = −4.6 ppm/°C. The microwave dielectric response of BNT-BSLT composite ceramics is closely related to the phase composition and defects, which is informative for the development of low dielectric loss ceramics.

研究领域: 材料科学 · 电子工程
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Excellent temperature stability of strain in PZ-PT-BNT ternary ceramics

Yuanshui Liu,Feng Luo,Denghui Jiang,Linzhuang Xing,Liwei Song,Zhimin Li

Lead-based Pb(Zr, Ti)O 3 ceramics have been widely applied in piezoelectric actuators, and yet high temperature stability and large strain have been pursued for further application. In this work, a novel PbZrO 3 –PbTiO 3 -(Bi 0.5 Na 0.5 )TiO 3 (PZ-PT-BNT) piezoelectric ceramic is designed and prepared by solid-state route. It is found that the introduction of BNT constituent enhances the relaxation behavior of PZ-PT ceramic, inhibits the abrupt change in dielectric properties near Curie temperature , and increases the proportion of tetragonal phase with high temperature stability. Meanwhile, the patterns of electric domains are intentionally modified by adjusting composition of PZ-PT-BNT. Short and broad electric domains in PZ-PT-0.03BNT ceramic are observed by piezoresponse force microscopy, which are insensitive to temperature and have faster response under electric field, contributing to strain characteristics. As a result, through integrating phase structure and electric domain configuration, a strain of 0.21% and excellent temperature stability where the variation of strain is less than 8% in the temperature range of 25–250 °C are achieved in PZ-PT-0.03BNT ceramic. The findings provide an effective strategy for improving the strain stability of PZ-PT-based piezoelectric ceramics, and demonstrate that PZ-PT-BNT ceramics have potential application prospects in high-temperature piezoelectric actuators.

研究领域: 材料科学 · 电子工程
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