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Article(id=1319973025357878078, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319973019079000285, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20230756, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1695916800000, receivedDateStr=2023-09-29, revisedDate=1699891200000, revisedDateStr=2023-11-14, acceptedDate=null, acceptedDateStr=null, onlineDate=1792635693157, onlineDateStr=2026-10-22, pubDate=1713542400000, pubDateStr=2024-04-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792635693157, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792635693157, creator=13701087609, updateTime=1792635693157, updator=13701087609, issue=Issue{id=1319973019079000285, tenantId=1146029695717560320, journalId=1263187385517883426, year='2024', volume='52', issue='4', pageStart='1171', pageEnd='1476', issueExtLink='null', onlineDate='null', pubDate='1713542400000', pubDateStr='2024-04-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792635691661, creator='13701087609', updateTime=1792641833008, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1319998777822396474, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319973019079000285, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1319998777822396475, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319973019079000285, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=1192, endPage=1199, ext={EN=ArticleExt(id=1319973027236926271, articleId=1319973025357878078, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Effect of Nd3+ Doping on Dielectric Properties and Energy Storage Properties of PLZS Antiferroelectrics, columnId=1321894869182828764, journalTitle=Journal of the Chinese Ceramic Society, columnName=Special Issue on Dielectric Energy Storage Materials—Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction

Ceramic-based dielectric capacitors with a high power density are one of the most prospective energy-storage components, compared with Li-ion batteries and super-capacitors. Unfortunately, the energy-storage density of ceramic-based dielectric capacitors is one or two orders of magnitude lower than that of the batteries, which is restricted by the property of dielectric materials. Therefore, developing reliable and high-performance dielectric ceramic is a challenge in the field of dielectric capacitors. Among dielectric ceramics, antiferroelectic (AFE) material is one of the most promising candidates for energy-storage devices since they show a high maximum polarization (Pmax), low remnant polarization (Pr), and a regulated AFE-ferroelectric (FE) phase transition electric field. Recent efforts are made to enhance energy-storage properties of ceramic by component design, ion-doping and material form construct. However, a superior η is always gained at the cost of a high Wrec, becoming a challenge for synergistically achieving a ultrahigh Wrec and a superior η.

Methods

High-purity Pb3O4 (≥95.0%, Sinopharm Chemical Reagent Co., Ltd., China), La2O3 (≥99.9%, Sinopharm Chemical Reagent Co., Ltd., China), Nd2O3 (>99.99%, Aladdin Biochemical Technology Co., Ltd., China), ZrO2 (≥99.0%, Sinopharm Chemical Reagent Co., Ltd., China), and SnO2 (≥99.5%, Sinopharm Chemical Reagent Co., Ltd.) were used as raw materials. Pb0.98-1.5xLa0.02Ndx(Zr0.60Sn0.40)0.995O3 (PL100xNZS) was selected as a basic system. Nd3+ with a small ionic radius (i.e., 1.29 Å) was introduced in PLZS to replace Pb2+ (i.e., 1.49 Å) for enhancing electric filed-induced EFE-AFE. A Pb0.98-1.5xLa0.02Ndx(Zr0.60Sn0.40)0.995O3 component was designed and the ceramics were fabricated by a tape-casting method.

The crystallinity, phase structure and microstructure of PL100xNZS ceramics were analyzed by an X-ray diffractometer (Rigaku Co., Ltd., Japan) and a model TESCAN-MIRA3 field-emission scanning electron microscope (TESCAN Co., Czech). The dielectric properties of the PL100xNZS ceramics were measured by a computer-controlled Agilent E4980A LCR analyzer. The displace-electric field (D-E) hysteresis loops and current density-electric field curve were determined by a ferroelectric measurement system (Radiant Technologies Co., USA). The pulsed charge-discharge behaviors were determined by a model CFD-001 resistance-inductance-capacitance (R-L-C) electric circuit (Guoguo Technology Co., China).

Results and discussion

The XRD patterns show that all the samples exhibit a perovskite structure with an orthorhombic phase. The SEM images show that a dense and compact microstructure appears in PL100xNZS ceramics. The average grain size is decreased by doping of Nd3+. The dielectric behavior of PL100xNZS ceramics as a function of temperature measured at 10 kHz and 25-400 ℃ indicates that there are three stages of dielectric constant with the increase of temperature, i.e., the rising, the plateau and the falling regions, which correspond to the AFE, multicell cubic (MCC) and single-cell cubic (PEC) phases. The maximum polarization decreases at the same electric field, and the breakdown strength (BDS) increases with the increase of Nd3+ content due to the decreased grain size. The antiferroelectric-ferroelectric phase transition electric field (EAFE-FE) increases as the Nd3+ content increases, because of a stable antiferroelectric phase. The enhanced BDS and increased EAFE-FE imply a high energy-storage density. The recoverable energy-storage density and efficiency are critical parameters to characterize the material performance. Herein, the PL4NZS ceramic can be used as a promising energy-storage material because it exhibits a linear-like D-E loop with a large Pmax (i.e., 60 μC/cm2) and a high BDS (i.e., 490 kV/cm). A large energy storage density of 14.8 J/cm3 is obtained in PL4NZS ceramic with a high efficiency of 85%. The calculated values of Wrec and η fluctuate slightly in the range of 6.18-4.88 J/cm3 with increasing the frequency. The discharge waveforms of PL4NZS ceramic at different electric fields are investigated at room temperature with an overdamped R-L-C electric circuit. The maximum value of Wdis is 4.4 J/cm3 at 300 kV/cm, and the t0.9 is 28 ns. A large CDmax of 3 360 A/cm2 and a high PDmax of 504 MW/cm3 are achieved at 300 kV/cm in PL4NZS ceramic, indicating that the PL4NZS ceramic has a great competitiveness in high power system applications.

Conclusions

The high energy-storage density and efficiency were realized in designed PL100xNZS ceramics fabricated by a tape-casting technique. The effects of Nd3+ doping on the microstructure, dielectric properties, ferroelectric properties and energy storage properties of the ceramics were investigated. The Wrec was 14.8 J/cm3 with a giant η of 85% at 490 kV/cm for PL4NZS ceramic. As the temperature increases, Wrec and η of PL4NZS ceramic increased slightly. Moreover, a high Wdis of 4.4 J/cm3, a large CDmax of 3 360 A/cm2 and a high PDmax of 504 MW/cm3 were obtained in PL4NZS ceramic. It was indicated that PL4NZS ceramic could be used as a prospective dielectric material for energy-storage applications.

, authors=Ande JIAO, Ye ZHAO, Pei HAN, Ninging SUN, Chunxiao LU, Jinhua DU, Yong LI, Qiwei ZHANG, Xihong HAO, authorsList=Ande JIAO, Ye ZHAO, Pei HAN, Ninging SUN, Chunxiao LU, Jinhua DU, Yong LI, Qiwei ZHANG, Xihong HAO, authorCompany=null, correspAuthors=Yong LI, Qiwei ZHANG, authorNote=

JIAO Ande (1999-), male, Master candidate. E-mail:

, correspAuthorsNote=
LI Yong (1982-), male, Ph.D., Professor. E-mail: ;
ZHANG Qiwei (1978-), male, Ph.D., Professor.
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近年来，随着科学技术的发展，高功率密度和快速充放电陶瓷引起了人们的广泛关注。采用流延法和固相烧结法制备了Pb0.98-1.5xLa0.02Ndx（Zr0.60Sn0.40）0.995O3（x=0，0.02，0.04，0.06，简写为PL100xNZS）反铁电陶瓷，并研究了反铁电陶瓷的相组成、储能性能、介电性能和充放电性能。研究结果表明：PL100xNZS的主晶相为正交相钙钛矿结构，随着Nd3+掺杂量的增多，反铁电-铁电相转变电场（EAFE-FE）增加，故其储能性能增强。当Nd3+掺杂量为x=0.04时，陶瓷的储能密度为14.8 J·cm-3，储能效率为85%。此外，充放电测试结果显示PL4NZS陶瓷具有高的电流密度和功率密度，分别为3 360 A/cm2和504 MW·cm-3，且放电速度极快，t0.9为28 ns。该结果表明PL4NZS材料在脉冲功率电容器领域具有重要的应用价值。

, authors=焦安德, 赵烨, 韩沛, 孙宁宁, 卢春晓, 杜金花, 李雍, 张奇伟, 郝喜红, authorsList=焦安德, 赵烨, 韩沛, 孙宁宁, 卢春晓, 杜金花, 李雍, 张奇伟, 郝喜红, authorCompany=null, correspAuthors=李雍, 张奇伟, authorNote=

焦安德（1999—），男，硕士研究生。

, correspAuthorsNote=
李雍（1982—），男，博士，教授；
张奇伟（1978—），男，博士，教授。
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Nd3+掺杂对PLZS反铁电体介电性能和储能性能的影响
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焦安德 , 赵烨 , 韩沛 , 孙宁宁 , 卢春晓 , 杜金花 , 李雍 , 张奇伟 , 郝喜红
硅酸盐学报 | 电介质储能材料专刊—研究论文 2024,52(4): 1192-1199
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硅酸盐学报 |电介质储能材料专刊—研究论文 2024 , 52 (4) : 1192 -1199
Nd3+掺杂对PLZS反铁电体介电性能和储能性能的影响
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焦安德 , 赵烨, 韩沛, 孙宁宁, 卢春晓, 杜金花, 李雍 , 张奇伟 , 郝喜红
作者信息
  • 内蒙古科技大学材料与冶金学院，内蒙古自治区铁电新能源材料与器件重点实验室，内蒙古 包头 014010
通讯作者:
李雍（1982—），男，博士，教授；
张奇伟（1978—），男，博士，教授。
作者简介:

焦安德（1999—），男，硕士研究生。

Effect of Nd3+ Doping on Dielectric Properties and Energy Storage Properties of PLZS Antiferroelectrics
Ande JIAO , Ye ZHAO, Pei HAN, Ninging SUN, Chunxiao LU, Jinhua DU, Yong LI , Qiwei ZHANG , Xihong HAO
Affiliations
  • Inner Mongolia Key Laboratory of Ferroelectric-Related New Energy Materials and Devices, School of Materials and Metallurgy, Inner Mongolia University of Science and Technology, Baotou 014010, China
    • Corresponding Author:
    LI Yong (1982-), male, Ph.D., Professor. E-mail: ;
    ZHANG Qiwei (1978-), male, Ph.D., Professor.

    JIAO Ande (1999-), male, Master candidate. E-mail:

出版时间: 2024-04-20 doi: 10.14062/j.issn.0454-5648.20230756
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近年来，随着科学技术的发展，高功率密度和快速充放电陶瓷引起了人们的广泛关注。采用流延法和固相烧结法制备了Pb0.98-1.5xLa0.02Ndx（Zr0.60Sn0.40）0.995O3（x=0，0.02，0.04，0.06，简写为PL100xNZS）反铁电陶瓷，并研究了反铁电陶瓷的相组成、储能性能、介电性能和充放电性能。研究结果表明：PL100xNZS的主晶相为正交相钙钛矿结构，随着Nd3+掺杂量的增多，反铁电-铁电相转变电场（EAFE-FE）增加，故其储能性能增强。当Nd3+掺杂量为x=0.04时，陶瓷的储能密度为14.8 J·cm-3，储能效率为85%。此外，充放电测试结果显示PL4NZS陶瓷具有高的电流密度和功率密度，分别为3 360 A/cm2和504 MW·cm-3，且放电速度极快，t0.9为28 ns。该结果表明PL4NZS材料在脉冲功率电容器领域具有重要的应用价值。

锆锡镧铅反铁电陶瓷  /  储能密度  /  介电性能  /  放电性能
Introduction

Ceramic-based dielectric capacitors with a high power density are one of the most prospective energy-storage components, compared with Li-ion batteries and super-capacitors. Unfortunately, the energy-storage density of ceramic-based dielectric capacitors is one or two orders of magnitude lower than that of the batteries, which is restricted by the property of dielectric materials. Therefore, developing reliable and high-performance dielectric ceramic is a challenge in the field of dielectric capacitors. Among dielectric ceramics, antiferroelectic (AFE) material is one of the most promising candidates for energy-storage devices since they show a high maximum polarization (Pmax), low remnant polarization (Pr), and a regulated AFE-ferroelectric (FE) phase transition electric field. Recent efforts are made to enhance energy-storage properties of ceramic by component design, ion-doping and material form construct. However, a superior η is always gained at the cost of a high Wrec, becoming a challenge for synergistically achieving a ultrahigh Wrec and a superior η.

Methods

High-purity Pb3O4 (≥95.0%, Sinopharm Chemical Reagent Co., Ltd., China), La2O3 (≥99.9%, Sinopharm Chemical Reagent Co., Ltd., China), Nd2O3 (>99.99%, Aladdin Biochemical Technology Co., Ltd., China), ZrO2 (≥99.0%, Sinopharm Chemical Reagent Co., Ltd., China), and SnO2 (≥99.5%, Sinopharm Chemical Reagent Co., Ltd.) were used as raw materials. Pb0.98-1.5xLa0.02Ndx(Zr0.60Sn0.40)0.995O3 (PL100xNZS) was selected as a basic system. Nd3+ with a small ionic radius (i.e., 1.29 Å) was introduced in PLZS to replace Pb2+ (i.e., 1.49 Å) for enhancing electric filed-induced EFE-AFE. A Pb0.98-1.5xLa0.02Ndx(Zr0.60Sn0.40)0.995O3 component was designed and the ceramics were fabricated by a tape-casting method.

The crystallinity, phase structure and microstructure of PL100xNZS ceramics were analyzed by an X-ray diffractometer (Rigaku Co., Ltd., Japan) and a model TESCAN-MIRA3 field-emission scanning electron microscope (TESCAN Co., Czech). The dielectric properties of the PL100xNZS ceramics were measured by a computer-controlled Agilent E4980A LCR analyzer. The displace-electric field (D-E) hysteresis loops and current density-electric field curve were determined by a ferroelectric measurement system (Radiant Technologies Co., USA). The pulsed charge-discharge behaviors were determined by a model CFD-001 resistance-inductance-capacitance (R-L-C) electric circuit (Guoguo Technology Co., China).

Results and discussion

The XRD patterns show that all the samples exhibit a perovskite structure with an orthorhombic phase. The SEM images show that a dense and compact microstructure appears in PL100xNZS ceramics. The average grain size is decreased by doping of Nd3+. The dielectric behavior of PL100xNZS ceramics as a function of temperature measured at 10 kHz and 25-400 ℃ indicates that there are three stages of dielectric constant with the increase of temperature, i.e., the rising, the plateau and the falling regions, which correspond to the AFE, multicell cubic (MCC) and single-cell cubic (PEC) phases. The maximum polarization decreases at the same electric field, and the breakdown strength (BDS) increases with the increase of Nd3+ content due to the decreased grain size. The antiferroelectric-ferroelectric phase transition electric field (EAFE-FE) increases as the Nd3+ content increases, because of a stable antiferroelectric phase. The enhanced BDS and increased EAFE-FE imply a high energy-storage density. The recoverable energy-storage density and efficiency are critical parameters to characterize the material performance. Herein, the PL4NZS ceramic can be used as a promising energy-storage material because it exhibits a linear-like D-E loop with a large Pmax (i.e., 60 μC/cm2) and a high BDS (i.e., 490 kV/cm). A large energy storage density of 14.8 J/cm3 is obtained in PL4NZS ceramic with a high efficiency of 85%. The calculated values of Wrec and η fluctuate slightly in the range of 6.18-4.88 J/cm3 with increasing the frequency. The discharge waveforms of PL4NZS ceramic at different electric fields are investigated at room temperature with an overdamped R-L-C electric circuit. The maximum value of Wdis is 4.4 J/cm3 at 300 kV/cm, and the t0.9 is 28 ns. A large CDmax of 3 360 A/cm2 and a high PDmax of 504 MW/cm3 are achieved at 300 kV/cm in PL4NZS ceramic, indicating that the PL4NZS ceramic has a great competitiveness in high power system applications.

Conclusions

The high energy-storage density and efficiency were realized in designed PL100xNZS ceramics fabricated by a tape-casting technique. The effects of Nd3+ doping on the microstructure, dielectric properties, ferroelectric properties and energy storage properties of the ceramics were investigated. The Wrec was 14.8 J/cm3 with a giant η of 85% at 490 kV/cm for PL4NZS ceramic. As the temperature increases, Wrec and η of PL4NZS ceramic increased slightly. Moreover, a high Wdis of 4.4 J/cm3, a large CDmax of 3 360 A/cm2 and a high PDmax of 504 MW/cm3 were obtained in PL4NZS ceramic. It was indicated that PL4NZS ceramic could be used as a prospective dielectric material for energy-storage applications.

PLZS antiferroelectric ceramics  /  energy storage density  /  dielectric properties  /  discharge performance
焦安德, 赵烨, 韩沛, 孙宁宁, 卢春晓, 杜金花, 李雍, 张奇伟, 郝喜红. Nd3+掺杂对PLZS反铁电体介电性能和储能性能的影响. 硅酸盐学报, 2024 , 52 (4) : 1192 -1199 . DOI: 10.14062/j.issn.0454-5648.20230756
Ande JIAO, Ye ZHAO, Pei HAN, Ninging SUN, Chunxiao LU, Jinhua DU, Yong LI, Qiwei ZHANG, Xihong HAO. Effect of Nd3+ Doping on Dielectric Properties and Energy Storage Properties of PLZS Antiferroelectrics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (4) : 1192 -1199 . DOI: 10.14062/j.issn.0454-5648.20230756
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  • 国家自然科学基金青年科学基金项目(52102136)
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doi: 10.14062/j.issn.0454-5648.20230756
  • 接收时间：2023-09-29
  • 首发时间：2026-10-22
  • 出版时间：2024-04-20
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  • 收稿日期：2023-09-29
  • 修回日期：2023-11-14
基金
国家自然科学基金青年科学基金项目(52102136)
作者信息
    内蒙古科技大学材料与冶金学院，内蒙古自治区铁电新能源材料与器件重点实验室，内蒙古 包头 014010

通讯作者:

李雍（1982—），男，博士，教授；
张奇伟（1978—），男，博士，教授。
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2种不同金属材料的力学参数
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
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