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Article(id=1319973033184449402, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319973019079000285, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20230742, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1695657600000, receivedDateStr=2023-09-26, revisedDate=1697990400000, revisedDateStr=2023-10-23, acceptedDate=null, acceptedDateStr=null, onlineDate=1792635695023, onlineDateStr=2026-10-22, pubDate=1713542400000, pubDateStr=2024-04-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792635695023, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792635695023, creator=13701087609, updateTime=1792635695023, 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=1183, endPage=1191, ext={EN=ArticleExt(id=1319973033465467771, articleId=1319973033184449402, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Effect of ZnO Doping on Energy Storage Properties of Strontium Titanate-Based Ceramics, 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

Dielectric capacitors are used in pulse power systems due to their advantages of high energy storage efficiency, long storage lifetime, and fast charge/discharge speed. Among the major dielectric materials, ceramic-based dielectrics have a superior temperature stability and a longer lifetime rather than polymer-based dielectrics. Dielectric energy storage ceramics have attracted recent attention. Among various dielectric energy storage ceramics, SrTiO3 ceramic with a linear dielectric behavior at room temperature is a promising dielectric energy storage material with a high breakdown strength and a low dielectric loss. However, SrTiO3 ceramic has a relatively low dielectric constant and lacks a spontaneous polarization, resulting in a limited energy storage density. Therefore, SrTiO3 ceramic cannot meet requirements for specific energy storage application. Improving the polarization strength while maintaining the high breakdown strength through effective structural adjustment can be an effective method to enhance its energy storage performance. In this paper, we fabricated high-performance (Sr0.42Na0.15Bi0.29Ca0.07□0.07)TiO3 (SNBCT) energy storage ceramics with a small amount of ZnO as doping species. In addition, the effect of ZnO doping on the structure and energy storage properties of the ceramics were also investigated.

Methods

SNBCT-x%ZnO energy storage ceramics were prepared by a conventional ceramic preparation process. The raw materials were weighed and then mixed in alcohol by grinding in a ball mill for 24 h. The slurry was dried and calcined at 950 ℃ for 4 h to obtain the powders. After further grinding for 24 h, the powders were mixed with polyvinyl alcohol (PVA) binder solution and then pressed into pellets with 10 mm in diameter and 0.5 mm in thickness. After burning off the PVA, the disk samples were sintered at 1 140 ℃ for 2 h. The samples used for dielectric performance tests were polished and coated with silver electrodes, and the samples used for energy storage and charge/discharge performance testing were thinned to a thickness of 0.1 mm, and gold electrodes with a diameter of 2 mm were sputtered on their surfaces.

The structure of the ceramic was analyzed by a model D8 advance X-ray diffractometer (Bruker Co., Germany). The microstructure of the ceramics was determined by a model Merlin compact field emission scanning electron microscope (Carl Zeiss Co., Germany). The ferroelectric properties of the ceramics were analyzed by a model TF Analyzer 3000 ferroelectric analyzer (aixACCT Co., Germany). The temperature-dependent dielectric properties were characterized by a model Wayne Kerr 6500B impedance analyzer (WayneKerr Co., UK). The charge-discharge characteristics were analyzed by a model CFD-003 plus pulsed charge-discharge system (Tongguo Technology Co., China).

Results and discussion

ZnO-modified SNBCT samples show a perovskite structure with a cubic phase. A trace of impurity peak appears in the XRD pattern as ZnO doping amount increases to 1.0%, corresponding to a small amount of the secondary Bi2Ti2O7 phase (JCPDS 032-0118). All the ceramics show a uniform and dense microstructure.

The ZnO doping has little influence on the microstructure of the ceramics as the average grain size in these compositions changes slightly.

For the electrical properties, the doping of ZnO weakens the ferroelectric properties of SNBCT ceramics, which is manifested by a decreased maximum polarization strength Pmax. In addition, the doping of ZnO improves the breakdown strength, thus enhancing the energy storage performance of SNBCT ceramics. For the sample doped with 0.5% ZnO, a high recoverable energy-storage density (Wrec) of 5.16 J/cm3 and a high energy-storage efficiency (η) of 88.2% in a large breakdown electric field of 468 kV/cm are obtained. Compared with the SrTiO3-based energy storage ceramics, a great energy storage performance of the studied sample is obtained. A simulation model containing grains and grain boundaries is proposed to explain the enhanced breakdown strength, and the results show that fine grains with many grain boundaries hinder the propagation of breakdown cracks. For the charge-discharge performance, the sample doped with 0.5% ZnO shows a discharge energy density (Wd) of 2.61 J/cm3 and a discharge rate (t0.9) of 227 ns in an electric field of 280 kV/cm.

Conclusions

All the samples exhibited a perovskite structure dominated by a cubic phase, and provided a slim P-E loops. ZnO doping effectively improved the breakdown strength of the SNBCT matrix, thus enhancing the energy storage performance. The effective energy storage density (Wrec) of the sample reached 5.16 J/cm3 and the energy storage efficiency (η) was 88.2% in the electric field of 468 kV/cm for the sample doped with 0.5% ZnO. A simulation model containing grains and grain boundaries was established and the extension of breakdown cracks in an external electric field was simulated, which explained the enhanced breakdown strength. In addition, the sample doped with 0.5% ZnO had a good charge-discharge performance, showing a discharge energy density (Wd) of 2.61 J/cm3 and a discharge rate (t0.9) of 227 ns in an electric field of 280 kV/cm. Meanwhile, the sample exhibited a good temperature stability. These results indicated that the SNBCT-x%ZnO ceramics could be promising materials for pulse power capacitor applications.

, authors=Jiarui WANG, Yang LIU, Lulu LIU, Di WANG, Chao WANG, Jigong HAO, Wei LI, authorsList=Jiarui WANG, Yang LIU, Lulu LIU, Di WANG, Chao WANG, Jigong HAO, Wei LI, authorCompany=null, correspAuthors=Jigong HAO, Wei LI, authorNote=

WANG Jiarui (2002-), female, Master candidate. E-mail:

, correspAuthorsNote=
HAO Jigong (1984-) male, Ph. D., Associate Professor. E-mail: ;
LI Wei (1981-) male, Ph. D., Professor.
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采用传统固相合成工艺制备了（Sr0.42Na0.15Bi0.29Ca0.07□0.07）TiO3-x%ZnO（□表示空位，化学式简写为SNBCT-x%ZnO，质量分数）储能陶瓷，并研究了ZnO掺杂对SNBCT陶瓷结构和储能性能的影响。结果表明：所用组分样品均具有以立方相为主相的钙钛矿结构，并表现出细长的电滞回线。ZnO掺杂有效提高了SNBCT陶瓷的击穿强度，并促进了其储能性能的提升。当ZnO掺杂量为0.5%时，样品在468 kV/cm电场下的有效储能密度（Wrec）达5.16 J/cm3，储能效率（η）为88.2%。通过有限元分析建立了该组分陶瓷的晶粒/晶界模型，模拟了电场作用下样品击穿裂纹的扩展，分析了样品高耐击穿行为的内在机理。此外，样品还具有良好的充放电性能，放电能量密度（Wd）和放电速率（t0.9）在280 kV/cm电场下分别为2.61 J/cm3和227 ns，同时样品表现出良好的温度稳定性，在脉冲功率系统中展示出良好的应用潜力。

, authors=王佳蕊, 刘洋, 刘璐璐, 王娣, 王超, 郝继功, 李伟, authorsList=王佳蕊, 刘洋, 刘璐璐, 王娣, 王超, 郝继功, 李伟, authorCompany=null, correspAuthors=郝继功, 李伟, authorNote=

王佳蕊（2002—），女，硕士研究生。

, correspAuthorsNote=
郝继功（1984—），男，博士，副教授。
李伟（1981—），男，博士，教授。
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ZnO掺杂对钛酸锶基陶瓷储能性能的影响
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王佳蕊 , 刘洋 , 刘璐璐 , 王娣 , 王超 , 郝继功 , 李伟
硅酸盐学报 | 电介质储能材料专刊—研究论文 2024,52(4): 1183-1191
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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) : 1183 -1191
ZnO掺杂对钛酸锶基陶瓷储能性能的影响
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王佳蕊 , 刘洋, 刘璐璐, 王娣, 王超, 郝继功 , 李伟
作者信息
  • 聊城大学材料科学与工程学院，山东省教育厅敏感材料与器件实验室，山东 聊城 252059
通讯作者:
郝继功（1984—），男，博士，副教授。
李伟（1981—），男，博士，教授。
作者简介:

王佳蕊（2002—），女，硕士研究生。

Effect of ZnO Doping on Energy Storage Properties of Strontium Titanate-Based Ceramics
Jiarui WANG , Yang LIU, Lulu LIU, Di WANG, Chao WANG, Jigong HAO , Wei LI
Affiliations
  • School of Materials Science and Engineering, Laboratory of Sensitive Materials and Devices Shandong Department of Education, Liaocheng University, Liaocheng 252059, Shandong, China
    • Corresponding Author:
    HAO Jigong (1984-) male, Ph. D., Associate Professor. E-mail: ;
    LI Wei (1981-) male, Ph. D., Professor.

    WANG Jiarui (2002-), female, Master candidate. E-mail:

出版时间: 2024-04-20 doi: 10.14062/j.issn.0454-5648.20230742
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摘要
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采用传统固相合成工艺制备了（Sr0.42Na0.15Bi0.29Ca0.07□0.07）TiO3-x%ZnO（□表示空位，化学式简写为SNBCT-x%ZnO，质量分数）储能陶瓷，并研究了ZnO掺杂对SNBCT陶瓷结构和储能性能的影响。结果表明：所用组分样品均具有以立方相为主相的钙钛矿结构，并表现出细长的电滞回线。ZnO掺杂有效提高了SNBCT陶瓷的击穿强度，并促进了其储能性能的提升。当ZnO掺杂量为0.5%时，样品在468 kV/cm电场下的有效储能密度（Wrec）达5.16 J/cm3，储能效率（η）为88.2%。通过有限元分析建立了该组分陶瓷的晶粒/晶界模型，模拟了电场作用下样品击穿裂纹的扩展，分析了样品高耐击穿行为的内在机理。此外，样品还具有良好的充放电性能，放电能量密度（Wd）和放电速率（t0.9）在280 kV/cm电场下分别为2.61 J/cm3和227 ns，同时样品表现出良好的温度稳定性，在脉冲功率系统中展示出良好的应用潜力。

电介质陶瓷  /  钛酸锶  /  储能性能  /  脉冲充放电
Introduction

Dielectric capacitors are used in pulse power systems due to their advantages of high energy storage efficiency, long storage lifetime, and fast charge/discharge speed. Among the major dielectric materials, ceramic-based dielectrics have a superior temperature stability and a longer lifetime rather than polymer-based dielectrics. Dielectric energy storage ceramics have attracted recent attention. Among various dielectric energy storage ceramics, SrTiO3 ceramic with a linear dielectric behavior at room temperature is a promising dielectric energy storage material with a high breakdown strength and a low dielectric loss. However, SrTiO3 ceramic has a relatively low dielectric constant and lacks a spontaneous polarization, resulting in a limited energy storage density. Therefore, SrTiO3 ceramic cannot meet requirements for specific energy storage application. Improving the polarization strength while maintaining the high breakdown strength through effective structural adjustment can be an effective method to enhance its energy storage performance. In this paper, we fabricated high-performance (Sr0.42Na0.15Bi0.29Ca0.07□0.07)TiO3 (SNBCT) energy storage ceramics with a small amount of ZnO as doping species. In addition, the effect of ZnO doping on the structure and energy storage properties of the ceramics were also investigated.

Methods

SNBCT-x%ZnO energy storage ceramics were prepared by a conventional ceramic preparation process. The raw materials were weighed and then mixed in alcohol by grinding in a ball mill for 24 h. The slurry was dried and calcined at 950 ℃ for 4 h to obtain the powders. After further grinding for 24 h, the powders were mixed with polyvinyl alcohol (PVA) binder solution and then pressed into pellets with 10 mm in diameter and 0.5 mm in thickness. After burning off the PVA, the disk samples were sintered at 1 140 ℃ for 2 h. The samples used for dielectric performance tests were polished and coated with silver electrodes, and the samples used for energy storage and charge/discharge performance testing were thinned to a thickness of 0.1 mm, and gold electrodes with a diameter of 2 mm were sputtered on their surfaces.

The structure of the ceramic was analyzed by a model D8 advance X-ray diffractometer (Bruker Co., Germany). The microstructure of the ceramics was determined by a model Merlin compact field emission scanning electron microscope (Carl Zeiss Co., Germany). The ferroelectric properties of the ceramics were analyzed by a model TF Analyzer 3000 ferroelectric analyzer (aixACCT Co., Germany). The temperature-dependent dielectric properties were characterized by a model Wayne Kerr 6500B impedance analyzer (WayneKerr Co., UK). The charge-discharge characteristics were analyzed by a model CFD-003 plus pulsed charge-discharge system (Tongguo Technology Co., China).

Results and discussion

ZnO-modified SNBCT samples show a perovskite structure with a cubic phase. A trace of impurity peak appears in the XRD pattern as ZnO doping amount increases to 1.0%, corresponding to a small amount of the secondary Bi2Ti2O7 phase (JCPDS 032-0118). All the ceramics show a uniform and dense microstructure.

The ZnO doping has little influence on the microstructure of the ceramics as the average grain size in these compositions changes slightly.

For the electrical properties, the doping of ZnO weakens the ferroelectric properties of SNBCT ceramics, which is manifested by a decreased maximum polarization strength Pmax. In addition, the doping of ZnO improves the breakdown strength, thus enhancing the energy storage performance of SNBCT ceramics. For the sample doped with 0.5% ZnO, a high recoverable energy-storage density (Wrec) of 5.16 J/cm3 and a high energy-storage efficiency (η) of 88.2% in a large breakdown electric field of 468 kV/cm are obtained. Compared with the SrTiO3-based energy storage ceramics, a great energy storage performance of the studied sample is obtained. A simulation model containing grains and grain boundaries is proposed to explain the enhanced breakdown strength, and the results show that fine grains with many grain boundaries hinder the propagation of breakdown cracks. For the charge-discharge performance, the sample doped with 0.5% ZnO shows a discharge energy density (Wd) of 2.61 J/cm3 and a discharge rate (t0.9) of 227 ns in an electric field of 280 kV/cm.

Conclusions

All the samples exhibited a perovskite structure dominated by a cubic phase, and provided a slim P-E loops. ZnO doping effectively improved the breakdown strength of the SNBCT matrix, thus enhancing the energy storage performance. The effective energy storage density (Wrec) of the sample reached 5.16 J/cm3 and the energy storage efficiency (η) was 88.2% in the electric field of 468 kV/cm for the sample doped with 0.5% ZnO. A simulation model containing grains and grain boundaries was established and the extension of breakdown cracks in an external electric field was simulated, which explained the enhanced breakdown strength. In addition, the sample doped with 0.5% ZnO had a good charge-discharge performance, showing a discharge energy density (Wd) of 2.61 J/cm3 and a discharge rate (t0.9) of 227 ns in an electric field of 280 kV/cm. Meanwhile, the sample exhibited a good temperature stability. These results indicated that the SNBCT-x%ZnO ceramics could be promising materials for pulse power capacitor applications.

dielectric ceramics  /  strontium titanate  /  energy storage performance  /  pulsed charge-discharge
王佳蕊, 刘洋, 刘璐璐, 王娣, 王超, 郝继功, 李伟. ZnO掺杂对钛酸锶基陶瓷储能性能的影响. 硅酸盐学报, 2024 , 52 (4) : 1183 -1191 . DOI: 10.14062/j.issn.0454-5648.20230742
Jiarui WANG, Yang LIU, Lulu LIU, Di WANG, Chao WANG, Jigong HAO, Wei LI. Effect of ZnO Doping on Energy Storage Properties of Strontium Titanate-Based Ceramics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (4) : 1183 -1191 . DOI: 10.14062/j.issn.0454-5648.20230742
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  • 山东省自然科学基金项目(ZR2020ME033; ZR2020ME031)
  • 聊城大学科研项目(318011906)
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doi: 10.14062/j.issn.0454-5648.20230742
  • 接收时间：2023-09-26
  • 首发时间：2026-10-22
  • 出版时间：2024-04-20
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  • 收稿日期：2023-09-26
  • 修回日期：2023-10-23
基金
山东省自然科学基金项目(ZR2020ME033; ZR2020ME031)
聊城大学科研项目(318011906)
作者信息
    聊城大学材料科学与工程学院，山东省教育厅敏感材料与器件实验室，山东 聊城 252059

通讯作者:

郝继功（1984—），男，博士，副教授。
李伟（1981—），男，博士，教授。
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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230742
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2种不同金属材料的力学参数
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Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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