Article(id=1321946043365839799, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1321945912352559151, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20250351, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1746460800000, receivedDateStr=2025-05-06, revisedDate=1749657600000, revisedDateStr=2025-06-12, acceptedDate=null, acceptedDateStr=null, onlineDate=1793106097308, onlineDateStr=2026-10-27, pubDate=1768838400000, pubDateStr=2026-01-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1793106097308, onlineIssueDateStr=2026-10-27, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1793106097308, creator=13701087609, updateTime=1793106097308, updator=13701087609, issue=Issue{id=1321945912352559151, tenantId=1146029695717560320, journalId=1263187385517883426, year='2026', volume='54', issue='1', pageStart='1', pageEnd='350', issueExtLink='null', onlineDate='null', pubDate='1767715200000', pubDateStr='2026-01-07', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1793106066072, creator='13701087609', updateTime=1793106066072, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext=null, issueFiles=null, downloadFileDto=null}, startPage=235, endPage=242, ext={EN=ArticleExt(id=1321946043558777784, articleId=1321946043365839799, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Energy Storage Properties of BaTiO3 Nanoparticle-Filled Sandwich-Structured Composite Films, columnId=1263922769897599102, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Articles, runingTitle=null, highlight=null, articleAbstract=
Introduction

The escalating demand for advanced energy storage systems in modern electronics, electric vehicles, and renewable power grids has propelled the development of high-performance dielectric capacitors. Among various types of capacitors, those based on polymer dielectrics are highly prized for their ultrahigh power density, low loss, and ability to operate at high voltages. However, a fundamental limitation of pure polymers is their relatively low dielectric constant, which constrains their energy storage density. A promising strategy to overcome this is to create composite materials that combine the high breakdown strength of polymers with the high dielectric constant of ceramic fillers. Sandwich-structured composites, in particular, have emerged as an ideal architecture. By strategically layering materials with complementary properties, it is possible to synergistically enhance both the dielectric constant and the breakdown strength, the two key parameters determining energy storage performance. Nevertheless, the design space for such multi-layered composites is vast and complex. Relying solely on experimental trial-and-error to optimize parameters like filler concentration and distribution is inefficient and costly. This study, therefore, aims to systematically design and theoretically investigate a novel sandwich-structured composite film. Using a phase-field model, we seek to elucidate the impact of critical microstructural parameters on the overall energy storage properties, providing a foundational guide for the experimental fabrication of next-generation high-energy-density capacitors.

Methods

A comprehensive phase-field model was developed to simulate the polarization response and dielectric breakdown behavior of the proposed sandwich-structured composite films. The modeled structure consisted of a three-layer film: two outer layers of polyetherimide (PEI), a polymer known for its high breakdown strength and thermal stability, and a central layer of polyvinylidene fluoride (PVDF), a polymer with a relatively high intrinsic dielectric constant. Barium titanate (BaTiO3, BT) nanoparticles, a classic ferroelectric ceramic with a very high dielectric constant, were incorporated as fillers exclusively within the central PVDF layer. This design intentionally confines the high-dielectric-constant ceramic phase to the middle layer, shielding it with the high-breakdown-strength PEI outer layers. The phase-field simulations accounted for key physical phenomena, including electric field distribution and the evolution of electrical treeing during breakdown. The primary variables investigated were the volume fraction of BT nanoparticles and their spatial dispersion uniformity within the PVDF matrix. The energy storage density of the materials was subsequently obtained through calculation of the simulation data.

Results and discussion

Simulation results revealed a non-monotonic relationship between the energy storage density and the volume fraction of BT nanoparticles. Initially, the energy storage performance enhanced with the addition of BT fillers. This improvement is attributed to the significant increase in the overall dielectric constant of the composite material due to the high dielectric constant of BT nanoparticles, enabling the storage of more charge under a given applied electric field. However, further increase in filler content led to deterioration in energy storage performance. This decline is primarily due to the formation of excessive interfacial areas between the polymer and ceramic phases and the increased likelihood of nanoparticle agglomeration. These interfaces create local field concentrations, which act as hotspots for premature electrical breakdown, thereby limiting the maximum applicable electric field. The trade-off between enhanced permittivity and reduced breakdown strength defines this optimal loading.

Furthermore, the study unequivocally demonstrated that the dispersion uniformity of the BT nanoparticles is a critical factor, often as important as the filler content itself. A heterogeneous, agglomerated distribution of nanoparticles resulted in severe local field distortion around the large clusters. These high-field regions became preferential paths for the initiation and propagation of breakdown channels, drastically reducing the overall dielectric strength of the composite. In contrast, a highly homogeneous dispersion of nanoparticles minimized local field concentrations, leading to a more uniform electric field distribution throughout the material. This uniformity allowed the composite to withstand much higher global electric fields before breakdown occurred, thereby maximizing the energy storage density. The results underscore that achieving a fine and uniform dispersion of nanofillers is paramount in material processing to realize the full potential of the composite design.

Conclusion

This work utilizes an advanced phase-field modeling framework to successfully design and analyze the energy storage performance of a PEI/PVDF-BT/PEI sandwich-structured composite film. The key conclusion is that both the volume fraction and the spatial distribution of ceramic nanofillers are decisive in determining the energy storage characteristics. An optimal BT nanoparticle volume fraction exists that balances the benefit of increased permittivity against the detriment of reduced breakdown strength. More significantly, a homogeneous dispersion of nanoparticles is crucial for mitigating local electric field concentrations and achieving a high breakdown strength. The findings provide profound insights and valuable quantitative guidance for the material-by-design of multilayer polymeric composites for high-energy-density capacitor applications.

, authors=Jiaqi WANG, Tengyue LIU, Yuliang ZHOU, Ben JIA, Peng ZHENG, authorsList=Jiaqi WANG, Tengyue LIU, Yuliang ZHOU, Ben JIA, Peng ZHENG, authorCompany=null, correspAuthors=Peng ZHENG, authorNote=

WANG Jiaqi (1999-), male, Master candidate. E-mail:

, correspAuthorsNote=
ZHENG Peng (1983-), male, Ph.D, Associate Professor. E-mail:
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介电电容器具有超高功率密度、低损耗以及高工作电压等优点,是广泛应用于电子电力系统的关键储能器件。三明治结构复合材料是发展高储能密度电介质材料的理想选择。然而三明治结构复合材料的设计复杂度明显提升,仅仅依靠实验很难获得最佳的组分。以聚醚酰亚胺作为外层,以聚偏二氟乙烯为中间层,以钛酸钡(BaTiO3,BT)为纳米填料构筑三明治结构复合薄膜,利用相场模拟探究了BT颗粒体积分数和分散度对三明治结构复合材料储能性能的影响。研究发现,随着BT体积分数的提高,复合薄膜的储能性能先提高后减少。此外,BT纳米颗粒的分散度对复合薄膜的储能性能有着明显的影响,纳米填料分布得越均匀,储能性能越好。最后,研究结果为三明治结构复合材料的设计提供了有价值的参考。

, authors=王嘉其, 刘腾岳, 周余粮, 贾犇, 郑鹏, authorsList=王嘉其, 刘腾岳, 周余粮, 贾犇, 郑鹏, authorCompany=null, correspAuthors=郑鹏, authorNote=

王嘉其(1999—),男,硕士研究生。

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郑鹏(1983—),男,博士,副教授。
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纳米钛酸钡填充三明治结构复合材料的储能性能
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王嘉其 , 刘腾岳 , 周余粮 , 贾犇 , 郑鹏
硅酸盐学报 | 研究论文 2026,54(1): 235-242
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硅酸盐学报 |研究论文 2026 , 54 (1) : 235 -242
纳米钛酸钡填充三明治结构复合材料的储能性能
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王嘉其 , 刘腾岳, 周余粮, 贾犇, 郑鹏
作者信息
  • 杭州电子科技大学电子科学与技术系纳米电子学与纳电子器件实验室,杭州 310018
通讯作者:
郑鹏(1983—),男,博士,副教授。
作者简介:

王嘉其(1999—),男,硕士研究生。

Energy Storage Properties of BaTiO3 Nanoparticle-Filled Sandwich-Structured Composite Films
Jiaqi WANG , Tengyue LIU, Yuliang ZHOU, Ben JIA, Peng ZHENG
Affiliations
  • Lab for Nanoelectronics and Nanoelectronic Devices, Department of Electronics Science and Technology, Hangzhou Dianzi University, Hangzhou 310018, China
  • Corresponding Author:
    ZHENG Peng (1983-), male, Ph.D, Associate Professor. E-mail:

    WANG Jiaqi (1999-), male, Master candidate. E-mail:

出版时间: 2026-01-20 doi: 10.14062/j.issn.0454-5648.20250351
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介电电容器具有超高功率密度、低损耗以及高工作电压等优点,是广泛应用于电子电力系统的关键储能器件。三明治结构复合材料是发展高储能密度电介质材料的理想选择。然而三明治结构复合材料的设计复杂度明显提升,仅仅依靠实验很难获得最佳的组分。以聚醚酰亚胺作为外层,以聚偏二氟乙烯为中间层,以钛酸钡(BaTiO3,BT)为纳米填料构筑三明治结构复合薄膜,利用相场模拟探究了BT颗粒体积分数和分散度对三明治结构复合材料储能性能的影响。研究发现,随着BT体积分数的提高,复合薄膜的储能性能先提高后减少。此外,BT纳米颗粒的分散度对复合薄膜的储能性能有着明显的影响,纳米填料分布得越均匀,储能性能越好。最后,研究结果为三明治结构复合材料的设计提供了有价值的参考。

纳米复合材料  /  相场模型  /  介电击穿  /  三明治结构
Introduction

The escalating demand for advanced energy storage systems in modern electronics, electric vehicles, and renewable power grids has propelled the development of high-performance dielectric capacitors. Among various types of capacitors, those based on polymer dielectrics are highly prized for their ultrahigh power density, low loss, and ability to operate at high voltages. However, a fundamental limitation of pure polymers is their relatively low dielectric constant, which constrains their energy storage density. A promising strategy to overcome this is to create composite materials that combine the high breakdown strength of polymers with the high dielectric constant of ceramic fillers. Sandwich-structured composites, in particular, have emerged as an ideal architecture. By strategically layering materials with complementary properties, it is possible to synergistically enhance both the dielectric constant and the breakdown strength, the two key parameters determining energy storage performance. Nevertheless, the design space for such multi-layered composites is vast and complex. Relying solely on experimental trial-and-error to optimize parameters like filler concentration and distribution is inefficient and costly. This study, therefore, aims to systematically design and theoretically investigate a novel sandwich-structured composite film. Using a phase-field model, we seek to elucidate the impact of critical microstructural parameters on the overall energy storage properties, providing a foundational guide for the experimental fabrication of next-generation high-energy-density capacitors.

Methods

A comprehensive phase-field model was developed to simulate the polarization response and dielectric breakdown behavior of the proposed sandwich-structured composite films. The modeled structure consisted of a three-layer film: two outer layers of polyetherimide (PEI), a polymer known for its high breakdown strength and thermal stability, and a central layer of polyvinylidene fluoride (PVDF), a polymer with a relatively high intrinsic dielectric constant. Barium titanate (BaTiO3, BT) nanoparticles, a classic ferroelectric ceramic with a very high dielectric constant, were incorporated as fillers exclusively within the central PVDF layer. This design intentionally confines the high-dielectric-constant ceramic phase to the middle layer, shielding it with the high-breakdown-strength PEI outer layers. The phase-field simulations accounted for key physical phenomena, including electric field distribution and the evolution of electrical treeing during breakdown. The primary variables investigated were the volume fraction of BT nanoparticles and their spatial dispersion uniformity within the PVDF matrix. The energy storage density of the materials was subsequently obtained through calculation of the simulation data.

Results and discussion

Simulation results revealed a non-monotonic relationship between the energy storage density and the volume fraction of BT nanoparticles. Initially, the energy storage performance enhanced with the addition of BT fillers. This improvement is attributed to the significant increase in the overall dielectric constant of the composite material due to the high dielectric constant of BT nanoparticles, enabling the storage of more charge under a given applied electric field. However, further increase in filler content led to deterioration in energy storage performance. This decline is primarily due to the formation of excessive interfacial areas between the polymer and ceramic phases and the increased likelihood of nanoparticle agglomeration. These interfaces create local field concentrations, which act as hotspots for premature electrical breakdown, thereby limiting the maximum applicable electric field. The trade-off between enhanced permittivity and reduced breakdown strength defines this optimal loading.

Furthermore, the study unequivocally demonstrated that the dispersion uniformity of the BT nanoparticles is a critical factor, often as important as the filler content itself. A heterogeneous, agglomerated distribution of nanoparticles resulted in severe local field distortion around the large clusters. These high-field regions became preferential paths for the initiation and propagation of breakdown channels, drastically reducing the overall dielectric strength of the composite. In contrast, a highly homogeneous dispersion of nanoparticles minimized local field concentrations, leading to a more uniform electric field distribution throughout the material. This uniformity allowed the composite to withstand much higher global electric fields before breakdown occurred, thereby maximizing the energy storage density. The results underscore that achieving a fine and uniform dispersion of nanofillers is paramount in material processing to realize the full potential of the composite design.

Conclusion

This work utilizes an advanced phase-field modeling framework to successfully design and analyze the energy storage performance of a PEI/PVDF-BT/PEI sandwich-structured composite film. The key conclusion is that both the volume fraction and the spatial distribution of ceramic nanofillers are decisive in determining the energy storage characteristics. An optimal BT nanoparticle volume fraction exists that balances the benefit of increased permittivity against the detriment of reduced breakdown strength. More significantly, a homogeneous dispersion of nanoparticles is crucial for mitigating local electric field concentrations and achieving a high breakdown strength. The findings provide profound insights and valuable quantitative guidance for the material-by-design of multilayer polymeric composites for high-energy-density capacitor applications.

nanocomposite  /  phase field model  /  dielectric breakdown  /  sandwich structure
王嘉其, 刘腾岳, 周余粮, 贾犇, 郑鹏. 纳米钛酸钡填充三明治结构复合材料的储能性能. 硅酸盐学报, 2026 , 54 (1) : 235 -242 . DOI: 10.14062/j.issn.0454-5648.20250351
Jiaqi WANG, Tengyue LIU, Yuliang ZHOU, Ben JIA, Peng ZHENG. Energy Storage Properties of BaTiO3 Nanoparticle-Filled Sandwich-Structured Composite Films[J]. Journal of the Chinese Ceramic Society, 2026 , 54 (1) : 235 -242 . DOI: 10.14062/j.issn.0454-5648.20250351
  • 浙江省自然科学基金(LY22E020006; LQ22A040012)
  • 浙江省属高校基础研究基金
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doi: 10.14062/j.issn.0454-5648.20250351
  • 接收时间:2025-05-06
  • 首发时间:2026-10-27
  • 出版时间:2026-01-20
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  • 收稿日期:2025-05-06
  • 修回日期:2025-06-12
基金
浙江省自然科学基金(LY22E020006; LQ22A040012)
浙江省属高校基础研究基金
作者信息
    杭州电子科技大学电子科学与技术系纳米电子学与纳电子器件实验室,杭州 310018

通讯作者:

郑鹏(1983—),男,博士,副教授。
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2种不同金属材料的力学参数
科
Family
属数
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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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