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Article(id=1210560431656144990, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1210560429043085661, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2024.07.004, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1688745600000, receivedDateStr=2023-07-08, revisedDate=1693324800000, revisedDateStr=2023-08-30, acceptedDate=null, acceptedDateStr=null, onlineDate=1766549698031, onlineDateStr=2025-12-24, pubDate=1721404800000, pubDateStr=2024-07-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1766549698031, onlineIssueDateStr=2025-12-24, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1766549698031, creator=13701087609, updateTime=1766549698031, updator=13701087609, issue=Issue{id=1210560429043085661, tenantId=1146029695717560320, journalId=1149653034449285133, year='2024', volume='57', issue='7', pageStart='1', pageEnd='142', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1766549697408, creator=13701087609, updateTime=1766563951127, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1210620213532430860, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1210560429043085661, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1210620213532430861, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1210560429043085661, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=28, endPage=35, ext={EN=ArticleExt(id=1210560432465645670, articleId=1210560431656144990, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Study on dielectric and energy storage characteristics of P(VDF-CTFE)/DA@BTO laminated composite film, columnId=1190369066675179686, journalTitle=Insulating Materials, columnName=Material Research, runingTitle=null, highlight=null, articleAbstract=

Polyvinylidene fluoride (PVDF)-based polymer has promising applications perspectives in the field of high energy storage density and high pulse energy storage. In this paper, barium titanate (BTO) nanoparticles were doped with polyvinylidene fluoride-chlorotrifluoroethylene (P(VDF-CTFE)) solution, and P(VDF-CTFE)/BTO composite films were prepared by solution casting method. The effects of different BTO doping contents on microstructure, dielectric properties, and energy storage characteristics of the composite films were investigated. Then the BTO was modified by dopamine (DA) to enhance the compatibility between BTO and polymer matrix and improve the dielectric constant and electric strength of composite films. At the same time, on the basis of the "breakdown blocking effect" between the films layers, the laminated composite films were prepared to enhance the energy storage properties. The results show that using the P(VDF-CTFE)/DA@BTO composite film with a DA modified BTO mass fraction of 10% as the interlayer, and the P(VDF-CTFE) as the outerlayer, the prepared PV-BT-PV laminated sandwich composite film has a dielectric constant of 10.44, a maximum electric strength of 362.25 kV/mm, and a charge discharge efficiency of 86.63% at an electric field strength of 500 kV/cm.

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聚偏氟乙烯（PVDF）基聚合物在高储能密度、高脉冲储能领域具有广泛的应用前景。本文采用钛酸钡（BTO）纳米颗粒掺杂聚偏氟乙烯-三氟氯乙烯（P(VDF-CTFE)）溶液，采用流延法制备P(VDF-CTFE)/BTO复合薄膜，探讨了不同BTO掺杂含量对复合薄膜微观结构、介电性能、储能特性的影响；采用多巴胺（DA）改性BTO以提升BTO与聚合物基体的相容性，改善复合薄膜的介电常数和电气强度；同时利用薄膜层间“击穿阻碍效应”制备层叠式结构复合薄膜以提升薄膜的储能特性。结果表明：使用DA改性BTO质量分数为10%的P(VDF-CTFE)/DA@BTO复合薄膜作为中间层、P(VDF-CTFE)作为外层制备的PV-BT-PV层叠式三明治结构复合薄膜，介电常数达到10.44，最大电气强度为362.25 kV/mm，在500 kV/cm电场强度下的充放电效率达到86.63%。

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熊平（1971-），女（汉族），四川简阳人，副教授，主要从事电子绝缘材料的研究。

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熊平（1971-），女（汉族），四川简阳人，副教授，主要从事电子绝缘材料的研究。

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熊平（1971-），女（汉族），四川简阳人，副教授，主要从事电子绝缘材料的研究。

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P(VDF-CTFE)/DA@BTO层叠式结构复合薄膜的介电与储能特性研究
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熊平 1 , 吴睿 2 , 马超 2 , 徐建华 4 , 王桥梅 3
绝缘材料 | 材料研究 2024,57(7): 28-35
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绝缘材料 | 材料研究 2024, 57(7): 28-35
P(VDF-CTFE)/DA@BTO层叠式结构复合薄膜的介电与储能特性研究
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熊平1, 吴睿2, 马超2, 徐建华4, 王桥梅3
作者信息
  • 1成都工业学院，材料与环境工程学院，四川 成都 611730
  • 2成都工业学院，电子工程学院，四川 成都 611730
  • 3成都工业学院，网络与通信工程学院，四川 成都 611730
  • 4电子科技大学 光电科学与工程学院，四川 成都 610054

    • 熊平（1971-），女（汉族），四川简阳人，副教授，主要从事电子绝缘材料的研究。

Study on dielectric and energy storage characteristics of P(VDF-CTFE)/DA@BTO laminated composite film
Ping XIONG1, Rui WU2, Chao MA2, Jianhua XU4, Qiaomei WANG3
Affiliations
  • 1School of Materials and Environmental Engineering, Chengdu Technological University, Chengdu 611730, China
  • 2School of Electronic Engineering, Chengdu Technological University, Chengdu 611730, China
  • 3School of Network & Communication Engineering, Chengdu Technological University, Chengdu 611730, China
  • 4School of Optoelectronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, China
出版时间: 2024-07-20 doi: 10.16790/j.cnki.1009-9239.im.2024.07.004
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聚偏氟乙烯（PVDF）基聚合物在高储能密度、高脉冲储能领域具有广泛的应用前景。本文采用钛酸钡（BTO）纳米颗粒掺杂聚偏氟乙烯-三氟氯乙烯（P(VDF-CTFE)）溶液，采用流延法制备P(VDF-CTFE)/BTO复合薄膜，探讨了不同BTO掺杂含量对复合薄膜微观结构、介电性能、储能特性的影响；采用多巴胺（DA）改性BTO以提升BTO与聚合物基体的相容性，改善复合薄膜的介电常数和电气强度；同时利用薄膜层间“击穿阻碍效应”制备层叠式结构复合薄膜以提升薄膜的储能特性。结果表明：使用DA改性BTO质量分数为10%的P(VDF-CTFE)/DA@BTO复合薄膜作为中间层、P(VDF-CTFE)作为外层制备的PV-BT-PV层叠式三明治结构复合薄膜，介电常数达到10.44，最大电气强度为362.25 kV/mm，在500 kV/cm电场强度下的充放电效率达到86.63%。

钛酸钡  /  聚偏氟乙烯-三氟氯乙烯  /  层叠式结构复合薄膜  /  介电特性  /  储能特性

Polyvinylidene fluoride (PVDF)-based polymer has promising applications perspectives in the field of high energy storage density and high pulse energy storage. In this paper, barium titanate (BTO) nanoparticles were doped with polyvinylidene fluoride-chlorotrifluoroethylene (P(VDF-CTFE)) solution, and P(VDF-CTFE)/BTO composite films were prepared by solution casting method. The effects of different BTO doping contents on microstructure, dielectric properties, and energy storage characteristics of the composite films were investigated. Then the BTO was modified by dopamine (DA) to enhance the compatibility between BTO and polymer matrix and improve the dielectric constant and electric strength of composite films. At the same time, on the basis of the "breakdown blocking effect" between the films layers, the laminated composite films were prepared to enhance the energy storage properties. The results show that using the P(VDF-CTFE)/DA@BTO composite film with a DA modified BTO mass fraction of 10% as the interlayer, and the P(VDF-CTFE) as the outerlayer, the prepared PV-BT-PV laminated sandwich composite film has a dielectric constant of 10.44, a maximum electric strength of 362.25 kV/mm, and a charge discharge efficiency of 86.63% at an electric field strength of 500 kV/cm.

BaTiO3  /  P(VDF-CTFE)  /  laminated composite film  /  dielectric characteristics  /  energy storage characteristics
熊平, 吴睿, 马超, 徐建华, 王桥梅. P(VDF-CTFE)/DA@BTO层叠式结构复合薄膜的介电与储能特性研究. 绝缘材料, 2024 , 57 (7) : 28 -35 . DOI: 10.16790/j.cnki.1009-9239.im.2024.07.004
Ping XIONG, Rui WU, Chao MA, Jianhua XU, Qiaomei WANG. Study on dielectric and energy storage characteristics of P(VDF-CTFE)/DA@BTO laminated composite film[J]. Insulating Materials, 2024 , 57 (7) : 28 -35 . DOI: 10.16790/j.cnki.1009-9239.im.2024.07.004
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0 引言
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静电薄膜电容器具有功率密度高、运行安全可靠性高等优点，被广泛应用于电动汽车、输变电系统、医疗设备、电磁弹射系统等领域[1]。但静电薄膜电容器的介电性能和储能性能较低，限制了其发展应用，因此提高其介电常数和储能特性成为研究重点。
目前广泛使用的聚丙烯（PP）膜介电常数较低（约为2.2），导致其储能密度不高（小于4 J/cm3），使得高储能应用场景下电容器的体积过大。针对目前高脉冲储能领域对电容器高储能密度的要求，使用更高介电常数的介质材料是满足这一要求的有效途径。
具有较高介电常数、电场强度以及优异柔韧性的聚偏氟乙烯（PVDF）基聚合物是储能领域非常具有潜力的电介质材料。以PVDF基聚合物为代表的极性高分子材料虽然具备较高的介电常数，但由于偶极子间的极化耦合带来巨大的能量损耗，导致其充放电效率较低。因此，解决介质膜储能密度与充放电效率的负相关性问题也成为了电介质材料储能领域的研究重点。研究者们为进一步提升与优化PVDF基聚合物的介电性能与储能特性，从分子结构、复合体系等方面开展了大量研究。V BHARTI等[2-4]通过电子射线辐射在聚合物中引入缺陷来提高其介电常数。XIE L Y等[5]将钛酸钡掺杂到聚合物基体中，并且在聚合物分子链上接枝GMA官能团，使复合薄膜的介电常数可提升至34.8（1 MHz）。ZHAO T等[6]对钛酸钡进行羟基化处理后与PVDF形成复合体系，氢键的加入在提升两相相容性的同时，也极大增强了材料的介电性能。
纳米复合是电介质材料性能优化的主要研究方向，研究者常将以钛酸钡（BaTiO3，BTO）为代表的无机纳米材料作为掺杂相引入到聚合物基体中。BTO凭借其超高的介电常数、优良的化学稳定性以及高机械强度等特点，在储能领域具有非常广泛的应用。同时，为了增强BTO在聚合物基体中的相容性与分散性，常利用硅烷偶联剂、磷酸、多巴胺等对BTO表面进行改性[7-10]。研究发现，大部分无机纳米材料的介电性能受温度和颗粒尺寸的影响较大[11]。温度越高，介电常数越高。随着纳米颗粒尺寸的减小，介电常数也会呈现先增大后减小的变化趋势[12]。因此，在有机/无机复合体系中，无机纳米颗粒尺寸的选择对复合材料性能的影响也是巨大的。
本文以聚偏氟乙烯-三氟氯乙烯（P(VDF-CTFE)）聚合物为基体材料，利用多巴胺对BTO纳米颗粒表面进行包覆改性，以提升聚合物基体与BTO纳米颗粒之间的相容性。采用溶液流延法制备层叠式结构复合薄膜，利用层间“击穿阻碍效应”提升薄膜的储能特性，同时探讨BTO掺杂量、多巴胺改性以及层叠式结构对复合薄膜介电和储能特性的影响，以期为探索高储能密度PVDF基电介质材料提供研究思路。
1 实验
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1.1 主要原材料
P(VDF-CTFE)购于索尔维（Solvay）公司，BTO纳米颗粒购于Sigma-Aldrich公司，盐酸多巴胺（化学纯）购于Alfa Aesar（中国）化学有限公司，N,N-二甲基甲酰胺（DMF）、氨水等溶剂（分析纯，99.8%）购于成都科隆化工试剂有限公司。
1.2 P(VDF-CTFE)/BTO薄膜的制备
称取1.0 g的P(VDF-CTFE)粉末加入烧杯中，再加入9.0 g的DMF溶剂和一定量的BTO纳米颗粒，机械搅拌10 h，待聚合物完全溶解后将烧杯置于真空烘箱（设定气压值为0.08 MPa）内真空除气2 h。然后，将溶液倾倒于洁净石英板表面，利用刮刀流延为液膜，再将石英板置于恒温加热台（60℃）加热10 h去除溶剂。最后，在200℃下退火20 min，在0℃冰水中淬火20 min，再将石英板置于70℃恒温加热台对薄膜进行干燥处理，最终得到复合薄膜。
1.3 P(VDF-CTFE)/DA@BTO复合薄膜的制备
为改善BTO与基体材料的相容性，首先制备了多巴胺包覆的BTO纳米颗粒。在pH值为8.5的稀氨水溶液中进行多巴胺氧化交联反应（如图1所示），自聚成具有强粘附性的高分子聚合物聚多巴胺[13]。随后向聚多巴胺碱性溶液加入BTO纳米颗粒，在弱碱性环境中，聚多巴胺的羟基（-OH）可以与BTO表面羟基脱水形成氢键，聚多巴胺通过键合作用在BTO表面形成核壳结构，使聚多巴胺包覆层可以有效提升BTO与P(VDF-CTFE)聚合物的相容性[14]。多巴胺改性BTO纳米颗粒的流程如图2所示。
采取同1.2节的成膜方法制备了P(VDF-CTFE)/DA@BTO复合薄膜。
1.4 P(VDF-CTFE)/DA@BTO层叠式结构复合薄膜的制备
按照上述薄膜制备方法逐层流延底层、中间层、上层薄膜，每层薄膜的流延均在下一层液膜溶剂完全挥发后进行流涎。通过控制液膜厚度使每层薄膜厚度保持在5 μm。如图3所示，分别以 P(VDF-CTFE)/DA@BTO复合薄膜与纯P(VDF-CTFE)作为中间层制备了两种层叠式三明治结构复合薄膜，并命名为PV-BT-PV、BT-PV-BT。
1.5 表征与性能测试
采用Hitachi公司生产的S-4800型扫描电子显微镜表征薄膜微观形貌，在薄膜两面蒸镀尺寸为1.2 cm×1.2 cm的铝电极用于后续介电储能特性测试。采用Agilent Technologies公司生产的4294A型阻抗分析仪测量薄膜在不同频率下的介电频谱特性。采用常州同惠电子有限公司生产的TH9201型耐压测试仪测量薄膜的击穿电压，升压速率为500 V/s。采用Radiant Technologies公司生产的铁电测试仪的Hysteresis模块（10 Hz，Standard monopolar）测试薄膜的充放电循环曲线，并计算薄膜的充放电效率与能量密度。
2 结果与讨论
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2.1 P(VDF-CTFE)/BTO复合薄膜的形貌及性能
2.1.1 表面形貌
图4为1 000放大倍率下掺杂BTO质量分数分别为5%、10%、15%、20%的P(VDF-CTFE)/BTO薄膜的表面形貌。从图4可以看出，BTO质量分数为5%、10%、15%的复合薄膜表面BTO颗粒大小均匀，致密度高，而BTO质量分数为20%的复合薄膜由于掺杂量较大，出现较大颗粒物，表面凹凸不平，平整度较差。
2.1.2 介电特性及储能特性
图5为掺杂不同BTO含量的P(VDF-CTFE)/BTO复合薄膜的介电频谱特性。从图5可以看出，随着BTO含量的增加，复合薄膜的介电常数、介质损耗因数均升高。在频率为500 Hz时，掺杂质量分数为20% BTO纳米颗粒的复合薄膜介电常数比掺杂质量分数为5% BTO的复合薄膜提升了51.32%。复合薄膜的介电常数随频率增加呈下降趋势，这是由于复合薄膜内部偶极矩在转向过程中受临近分子碰撞导致转向速率滞后于交变电场的变化速率，即介电弛豫现象[15]。复合薄膜的介质损耗因数随频率增加呈先减小后增大的趋势。在低频率下，BTO掺杂含量对复合薄膜的介质损耗影响很小；在高频率下，受弛豫影响介质损耗急速增加，且BTO掺杂含量越高，介质损耗越大。原因在于随着聚合物中BTO含量增加，复合薄膜易产生空洞、裂纹以及颗粒团聚等现象[16]。因此，无机纳米颗粒的添加有利于提升复合薄膜的介电常数。
图6为掺杂不同BTO含量的P(VDF-CTFE)/BTO复合薄膜的击穿特性威布尔（Weibull）分布。二参数威布尔方程如式（1）所示。
P(E)=1-exp (-EEbβ)
式（1）中：P(E)为电介质的累计击穿概率；E为外加电气强度；Eb为尺度参数，代表电介质累计击穿概率达63.2%时的特征电气强度，通常用此参数来表征电介质的电气强度；β为形状参数，用于分析数据的离散状况。
根据IEEE 930-2004相关规定，电介质材料的击穿概率可由式（2）计算。
Pi=i-0.44n+0.25×100%
式（2）中，i代表将n个金属化点测量得到的电气强度值E按从小到大顺序排列后的第i个结果，本次实验中n=16。
数据处理过程中，计算lg(-ln(1-Pi))与lgEi值，并以lgEi为自变量，对lg(-ln(1-Pi))作图，将数据进行线性拟合得出形状参数β即直线斜率。取lg(-ln(1-Pi))=0直线与拟合直线的交点，得到对应横坐标特征值，由此可计算材料的特征电气强度Eb。从图6可以看出，复合薄膜的电气强度随着BTO含量的增加呈显著下降趋势。当BTO质量分数为5%时，复合薄膜的电气强度为25.951 kV/mm，相对于纯聚合物薄膜（40.902 kV/mm）下降了36.55%；当BTO质量分数为20%时，电气强度下降至15.792 kV/mm，相对于纯聚合物薄膜下降了61.39%。这是由于BTO的加入造成了微孔结构缺陷，导致薄膜易于局部击穿；同时，掺杂BTO使得两相界面间形成导电通道，降低了击穿阈值，导致复合薄膜的耐压性能降低。
图7为掺杂不同BTO含量的复合薄膜的单向电滞回线（P-E）。从图7可以看出，随着BTO含量的增加，纳米颗粒在基体中引入大量界面极化，导致复合薄膜的最大极化强度升高，同时引入BTO导致薄膜内部产生大量缺陷，提升了复合薄膜内部载流子迁移率，导致复合薄膜的漏导损耗显著增加。
图8为掺杂不同BTO含量的P(VDF-CTFE)/BTO复合薄膜的充放电效率。从图8可以看出，复合薄膜的充放电效率随着BTO含量的增加呈逐步下降的趋势。当BTO质量分数为5%时，复合薄膜在500 kV/cm电场强度下的充放电效率为81.23%；当BTO质量分数为20%时，复合薄膜在500 kV/cm电场强度下的充放电效率仅为74.79%，相较于BTO质量分数为5%时的复合薄膜下降了6.44%。在相同BTO含量下，随着电场强度的增大，复合薄膜的充放电效率明显降低。当电场强度增大到2 000 kV/cm时，BTO质量分数为5%的复合薄膜充放电效率下降至45.68%；BTO质量分数为20%的复合薄膜充放电效率急剧下降至22.36%。这是由于高BTO掺杂含量的复合薄膜内部形成了大量载流子迁移通道，导致漏导损耗巨大，能量损失严重。
综上可得，BTO掺杂含量越高，复合薄膜的介电常数提升越显著，但电气强度以及充放电效率会因过高掺杂含量而迅速下降。当BTO质量分数为10%时，其对复合薄膜整体的储能特性具有较好的提升效果。
2.2 P(VDF-CTFE)/DA@BTO复合薄膜的形貌及性能
2.2.1 表面形貌
图9为5 000放大倍率下掺杂BTO质量分数为10%、经多巴胺改性前后复合薄膜的表面形貌。从图9可以看出，P(VDF-CTFE)/BTO复合薄膜存在团聚现象，BTO颗粒在聚合物中分布不均匀，导致表面形貌粗糙；而P(VDF-CTFE)/DA@BTO复合薄膜表面平整，BTO颗粒分布均匀，成膜较好，表明多巴胺能有效改善有机物与无机物的界面相容性。
2.2.2 介电特性及储能特性
图10为掺杂不同含量BTO、经多巴胺改性前后复合薄膜的介电常数测试结果。从图10可以看出，经过多巴胺表面改性的BTO可以进一步提升薄膜的介电常数，原因在于BTO经多巴胺改性后，在基体中分布更均匀，纳米颗粒与基体的界面增多，额外引入的界面极化进一步提升了复合薄膜的介电常数。
图11为掺杂不同含量BTO、经多巴胺改性前后复合薄膜的电气强度。从图11可以看出，在相同BTO含量下，P(VDF-CTFE)/DA@BTO复合薄膜的电气强度明显高于P(VDF-CTFE)/BTO复合薄膜。一方面BTO表面的聚多巴胺提高了两相界面间的相容性，减少了颗粒掺杂引入的内部缺陷，提升了复合薄膜的耐压性能。另一方面复合薄膜的击穿机理是外加电场引起BTO材料内部自由电子与电介质分子碰撞激发出更多自由电子，导致电介质击穿[17]，而聚多巴胺提高了BTO与聚合物的结合度，降低了颗粒表面可移动电荷浓度，抑制了电荷迁移，从而提高了薄膜的电气强度[18]。
图12为掺杂BTO质量分数为10%、经多巴胺改性前后复合薄膜的P-E曲线。从图12可以看出，P(VDF-CTFE)/DA@BTO复合薄膜的最大极化程度高于P(VDF-CTFE)/BTO复合薄膜，这主要得益于分散得更好的BTO纳米颗粒引入了更多的界面极化，同时，剩余极化也低于P(VDF-CTFE)/BTO复合薄膜。
图13为掺杂BTO质量分数为10%、经多巴胺改性前后复合薄膜的充放电效率。由图13可知， P(VDF-CTFE)/DA@BTO复合薄膜的充放电效率明显高于P(VDF-CTFE)/BTO复合薄膜，原因在于BTO经多巴胺改性后，两相界面相容性提升，减少了BTO掺杂带来的内部缺陷，进而降低了复合薄膜的能量损耗。
综上所述，通过多巴胺改性BTO，提高了薄膜内两相界面间的相容性，因此P(VDF-CTFE)/DA@BTO复合薄膜的介电常数、电气强度和充放电效率均优于P(VDF-CTFE)/BTO复合薄膜。
2.3 P(VDF-CTFE)/DA@BTO层叠式结构复合薄膜的介电和储能特性
图14为不同结构复合薄膜的介电频谱特性，4种复合薄膜的厚度均控制在（15±1） μm。从图14可以看出，4种复合薄膜的介电常数从大到小排序依次为BT-PV-BT层叠式结构复合薄膜（11.63）、单层P(VDF-CTFE)/DA@BTO复合薄膜（11.40）、PV-BT-PV层叠式结构复合薄膜（10.44）、单层P(VDF-CTFE)复合薄膜（8.07）。由此表明，叠层结构薄膜同样具有较高的介电常数，特别是BT-PV-BT结构，层间界面极化的产生使得复合薄膜介电常数提升非常明显，同时保持了较低的介质损耗。
图15为不同结构复合薄膜的击穿特性。从图15可以看出，复合薄膜的电气强度从大到小排序依次为单层P(VDF-CTFE)薄膜（409.12 kV/mm）、PV-BT-PV层叠式三明治结构复合薄膜（362.25 kV/mm）、BT-PV-BT层叠式三明治结构复合薄膜（355.40 kV/mm）、单层P(VDF-CTFE)/DA@BTO薄膜（275.23 kV/mm），两种层叠式结构复合薄膜的电气强度均有大幅提高，相比单层P(VDF-CTFE)/DA@BTO薄膜分别提升了28.8%和31.5%。图16为击穿阻碍示意图，层叠式三明治结构可以利用层间“击穿阻碍效应”，即击穿方向会在层间交界处发生转折，产生一定距离横向击穿通道，从而在保证高介电常数的同时有效提高了电气强度。
图17为不同结构复合薄膜的充放电效率变化曲线。从图17可以看出，复合薄膜的充放电效率从大到小排序依次为单层P(VDF-CTFE)薄膜、PV-BT-PV层叠式三明治结构复合薄膜、BT-PV-BT层叠式三明治结构复合薄膜、单层P(VDF-CTFE)/DA@BTO薄膜。在500 kV/cm电场强度下，PV-BT-PV层叠式三明治结构复合薄膜的充放电效率为86.63%，略低于单层P(VDF-CTFE)薄膜的充放电效率87.7%，表明层叠式三明治结构可有效提升复合薄膜的充放电效率。
综上所述，PV-BT-PV层叠式三明治结构复合薄膜在保证高介电常数、高电气强度的同时提升了充放电效率，显著改善了复合薄膜的储能特性。
3 结论
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（1）综合考虑BTO掺杂含量对复合薄膜的介电常数、电气强度、储能特性的影响，选择BTO质量分数为10%，有助于改善复合薄膜整体的储能特性。
（2）采用多巴胺改性BTO，提高了BTO与薄膜基材界面间相容性，提升了P(VDF-CTFE)/DA@BTO复合薄膜的介电特性和储能特性。
（3）PV-BT-PV、BT-PV-BT层叠式三明治结构复合薄膜可以利用层间“击穿阻碍效应”，有效提升复合薄膜的电气强度，改善储能特性。其中PV-BT-PV三明治结构复合薄膜介电常数达到10.44，最大电气强度为362.25 kV/mm，在500 kV/cm电场强度下的充放电效率可达86.63%。
基金
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  • 国家自然科学基金资助项目(61904020)
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2024年第57卷第7期
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doi: 10.16790/j.cnki.1009-9239.im.2024.07.004
  • 接收时间：2023-07-08
  • 首发时间：2025-12-24
  • 出版时间：2024-07-20
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  • 收稿日期：2023-07-08
  • 修回日期：2023-08-30
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国家自然科学基金资助项目(61904020)
作者信息
    1成都工业学院，材料与环境工程学院，四川 成都 611730
    2成都工业学院，电子工程学院，四川 成都 611730
    3成都工业学院，网络与通信工程学院，四川 成都 611730
    4电子科技大学 光电科学与工程学院，四川 成都 610054
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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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红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
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