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Article(id=1198667701708222618, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1198667701179740314, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2023.05.009, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1649433600000, receivedDateStr=2022-04-09, revisedDate=1657123200000, revisedDateStr=2022-07-07, acceptedDate=null, acceptedDateStr=null, onlineDate=1763714250256, onlineDateStr=2025-11-21, pubDate=1684512000000, pubDateStr=2023-05-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1763714250256, onlineIssueDateStr=2025-11-21, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1763714250256, creator=13701087609, updateTime=1763714250256, updator=13701087609, issue=Issue{id=1198667701179740314, tenantId=1146029695717560320, journalId=1149653034449285133, year='2023', volume='56', issue='5', pageStart='1', pageEnd='113', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1763714250130, creator=13701087609, updateTime=1766563551357, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1210618536771318327, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1198667701179740314, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1210618536771318328, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1198667701179740314, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=55, endPage=62, ext={EN=ArticleExt(id=1198667701947297948, articleId=1198667701708222618, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Ageing characteristics of metallized film capacitor under ultra-high DC field, columnId=1190369198472794288, journalTitle=Insulating Materials, columnName=Insulation Technology, runingTitle=null, highlight=null, articleAbstract=

In order to reveal the ageing characteristics of metallized film capacitor under ultra-high DC field, the capacitor and its dielectric material were studied. On the basis of the practical working conditions of capacitor, the special designed capacitor elements were conducted ageing tests at 60℃ under the DC field of 0En, 1.4En, 1.5En, and 1.6En, respectively. The capacity of the capacitor elements during ageing and the base film (biaxially oriented polypropylene (BOPP) film) after ageing failure were tested. The results show that the failure mechanism of the capacitor is related to the ageing electric field, and there is an electric field threshold. When the ageing electric field is lower than the electric field threshold, the capacitor will go through a long-term failure, and its capacitance decreases affected by the performance degradation of film, the electrical strength of the film decreases with the decrease of the activation energy of molecular segment motion. When the ageing electric field is higher than the electric field threshold, the capacitor will go through a short-term failure, and the extremely high electrical stress causes the original weakness to break down rapidly, the self-healing area increases rapidly, so the equipment life is greatly shortened.

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为揭示超高直流电场作用下金属化膜电容器的老化特性，对电容器设备及其介质材料进行了研究。基于电容器的实际运行工况，对特殊设计的电容器元件在60℃下分别开展了直流场强为0En、1.4En、1.5En与1.6En的老化试验。对老化中的电容器元件电容量和老化失效后的基膜（双向拉伸聚丙烯（BOPP）薄膜）进行测试。结果表明：电容器失效机理与老化电场有关，存在阈值电场。当老化电场低于阈值电场时，电容器发生长期失效，受到薄膜性能劣化的影响电容量降低，薄膜的电气强度随分子链段运动活化能的降低而降低；当老化电场高于阈值电场时，电容器发生短期故障，极高的电应力使薄膜介质原有的电弱点迅速击穿，自愈面积快速增大，设备寿命大幅缩短。

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刘文凤（1982-），女（汉族），天津人，教授，主要从事先进介质材料的理论与应用研究。
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徐哲（1996-），女（汉族），河北保定人，硕士生，主要从事金属化膜电容器老化的研究。

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徐哲（1996-），女（汉族），河北保定人，硕士生，主要从事金属化膜电容器老化的研究。

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徐哲（1996-），女（汉族），河北保定人，硕士生，主要从事金属化膜电容器老化的研究。

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language=EN, label=Fig.14, caption=Capacitances of capacitors versus time, figureFileSmall=Es2ZeRyiPvLuwAeXGmG+kw==, figureFileBig=zqjooE6fCBtPbLA+QPU41w==, tableContent=null), ArticleFig(id=1210986428704625336, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1198667701708222618, language=CN, label=图14, caption=电容器电容量随时间的下降趋势, figureFileSmall=Es2ZeRyiPvLuwAeXGmG+kw==, figureFileBig=zqjooE6fCBtPbLA+QPU41w==, tableContent=null), ArticleFig(id=1210986428767539897, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1198667701708222618, language=EN, label=Tab.1, caption=Melting and crystallization temperature of BOPP films, figureFileSmall=null, figureFileBig=null, tableContent=
试样Tm/℃Xc/%
BOPP0170.1953.90
BOPP1169.2753.56
BOPP2170.5454.03
BOPP3169.2053.72
), ArticleFig(id=1210986428847231674, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1198667701708222618, language=CN, label=表1, caption=

BOPP薄膜的熔融温度和结晶温度

, figureFileSmall=null, figureFileBig=null, tableContent=
试样Tm/℃Xc/%
BOPP0170.1953.90
BOPP1169.2753.56
BOPP2170.5454.03
BOPP3169.2053.72
), ArticleFig(id=1210986428914340539, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1198667701708222618, language=EN, label=Tab.2, caption=DC electric strength under different breakdown probabilities of films, figureFileSmall=null, figureFileBig=null, tableContent=
项目BOPP0BOPP1BOPP2BOPP3
5%击穿概率对应的电气强度/(kV/mm)270.1322.9330.0339.7
63.2%击穿概率对应的电气强度/(kV/mm)555.7525.0565.9576.1
), ArticleFig(id=1210986428973060796, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1198667701708222618, language=CN, label=表2, caption=

薄膜试样不同击穿概率下的直流电气强度

, figureFileSmall=null, figureFileBig=null, tableContent=
项目BOPP0BOPP1BOPP2BOPP3
5%击穿概率对应的电气强度/(kV/mm)270.1322.9330.0339.7
63.2%击穿概率对应的电气强度/(kV/mm)555.7525.0565.9576.1
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超高直流电场作用下金属化膜电容器的老化特性
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徐哲 1 , 程璐 1 , 刘宏博 1 , 王镜然 1 , 马宇威 1 , 李志元 1 , 刘文凤 1 , 国江 2
绝缘材料 | 绝缘技术 2023,56(5): 55-62
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绝缘材料 | 绝缘技术 2023, 56(5): 55-62
超高直流电场作用下金属化膜电容器的老化特性
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徐哲1, 程璐1, 刘宏博1, 王镜然1, 马宇威1, 李志元1, 刘文凤1, 国江2
作者信息
  • 1西安交通大学 电力设备电气绝缘国家重点实验室,陕西 西安 710049
  • 2中国电力科学研究院有限公司 电网环境保护国家重点实验室,湖北 武汉 430074

    • 徐哲（1996-），女（汉族），河北保定人，硕士生，主要从事金属化膜电容器老化的研究。

通讯作者:

刘文凤（1982-），女（汉族），天津人，教授，主要从事先进介质材料的理论与应用研究。
Ageing characteristics of metallized film capacitor under ultra-high DC field
Zhe XU1, Lu CHENG1, Hongbo LIU1, Jingran WANG1, Yuwei MA1, Zhiyuan LI1, Wenfeng LIU1, Jiang GUO2
Affiliations
  • 1State Key Laboratory of Power Equipment and Electrical Insulation, Xi′an Jiaotong University, Xi′an 714009, China
  • 2State Key Laboratory of Power Grid Environmental Protection, China Electric Power Research Institute Co., Ltd., Wuhan 430074, China
出版时间: 2023-05-20 doi: 10.16790/j.cnki.1009-9239.im.2023.05.009
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摘要
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为揭示超高直流电场作用下金属化膜电容器的老化特性，对电容器设备及其介质材料进行了研究。基于电容器的实际运行工况，对特殊设计的电容器元件在60℃下分别开展了直流场强为0En、1.4En、1.5En与1.6En的老化试验。对老化中的电容器元件电容量和老化失效后的基膜（双向拉伸聚丙烯（BOPP）薄膜）进行测试。结果表明：电容器失效机理与老化电场有关，存在阈值电场。当老化电场低于阈值电场时，电容器发生长期失效，受到薄膜性能劣化的影响电容量降低，薄膜的电气强度随分子链段运动活化能的降低而降低；当老化电场高于阈值电场时，电容器发生短期故障，极高的电应力使薄膜介质原有的电弱点迅速击穿，自愈面积快速增大，设备寿命大幅缩短。

金属化膜电容器  /  BOPP  /  直流电老化

In order to reveal the ageing characteristics of metallized film capacitor under ultra-high DC field, the capacitor and its dielectric material were studied. On the basis of the practical working conditions of capacitor, the special designed capacitor elements were conducted ageing tests at 60℃ under the DC field of 0En, 1.4En, 1.5En, and 1.6En, respectively. The capacity of the capacitor elements during ageing and the base film (biaxially oriented polypropylene (BOPP) film) after ageing failure were tested. The results show that the failure mechanism of the capacitor is related to the ageing electric field, and there is an electric field threshold. When the ageing electric field is lower than the electric field threshold, the capacitor will go through a long-term failure, and its capacitance decreases affected by the performance degradation of film, the electrical strength of the film decreases with the decrease of the activation energy of molecular segment motion. When the ageing electric field is higher than the electric field threshold, the capacitor will go through a short-term failure, and the extremely high electrical stress causes the original weakness to break down rapidly, the self-healing area increases rapidly, so the equipment life is greatly shortened.

metallized film capacitor  /  BOPP  /  DC ageing
徐哲, 程璐, 刘宏博, 王镜然, 马宇威, 李志元, 刘文凤, 国江. 超高直流电场作用下金属化膜电容器的老化特性. 绝缘材料, 2023 , 56 (5) : 55 -62 . DOI: 10.16790/j.cnki.1009-9239.im.2023.05.009
Zhe XU, Lu CHENG, Hongbo LIU, Jingran WANG, Yuwei MA, Zhiyuan LI, Wenfeng LIU, Jiang GUO. Ageing characteristics of metallized film capacitor under ultra-high DC field[J]. Insulating Materials, 2023 , 56 (5) : 55 -62 . DOI: 10.16790/j.cnki.1009-9239.im.2023.05.009
正文
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0 引言
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金属化膜电容器是柔性直流输电系统的核心设备，起着稳定电压、过滤谐波的重要作用[1]。在金属化膜电容器运行过程中长期承受着超高直流电场，运行场强可达200 kV/mm[2]，在电、热、力多物理场耦合的作用下，其实际使用寿命仅为传统电容器的1/3。目前我国金属化膜电容器全部依赖于进口，是明显的“卡脖子”问题[3]。超高直流电场是造成金属化膜电容器失效的关键因素，因此研究超高直流电场作用下金属化膜电容器的老化特性及机理对于提升其可靠性具有重要意义。
迄今，关于电容器老化研究中的老化场强通常远低于金属化膜电容器的工作场强[4-6]。B GOSSE等[7]对在单/二苄基甲苯（M/DBT）中浸渍的BOPP薄膜进行了老化研究，指出当老化场强为135 kV/mm左右时，PP薄膜的降解主要来源于氧化。对于高场强作用下的电容器研究通常针对的是金属化膜脉冲电容器，LI H等[8-9]对金属化膜电容器在脉冲电压作用下的寿命进行了系列研究，结果表明增大金属化膜的方阻和层间压力均有利于提高其使用寿命，然而脉冲电容器通常不能长时间承受高场强。
本研究基于金属化膜电容器的实际运行温度及场强，通过设计特殊的“混合介质”结构电容器元件，研究超高直流电场作用下金属化膜电容器的失效规律及双向拉伸聚丙烯（BOPP）薄膜的劣化机理。该“混合介质”电容器元件由BOPP和金属化BOPP卷绕而成。一方面可以模拟BOPP薄膜在实际运行过程中的层间压强、薄膜张力、空气环境等条件；另一方面便于拆解出完整的BOPP薄膜进行理化测试分析。首先对“混合介质”电容器单元进行直流电老化试验，获得容量衰减曲线，然后对从失效电容器中拆解得到的BOPP薄膜进行红外光谱、凝胶渗透色谱、X射线衍射、差示扫描量热分析、动态热机械分析和直流击穿试验等测试，最终得到超高直流电场作用下金属化膜电容器的失效规律及其介质材料的劣化机理，为金属化膜电容器的优化设计及可靠性提升提供依据。
1 试验
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1.1 样品电容器元件
常规金属化膜电容器元件的基本结构如图1(a)所示，是由两层单面蒸镀金属层的BOPP薄膜交错叠放绕芯轴卷绕，并在两端喷金而制成[10]。一端的喷金层只与其中一层BOPP薄膜的金属层相接，从而实现电容器电极引线的连接。本研究设计的“混合介质”结构干式金属化膜电容器元件如图1(b)所示，与常规电容器相比，该电容器的金属化薄膜多叠加了一层BOPP薄膜。
对图1(b)所示结构采用环氧树脂浇注并用塑料封装得到如图2所示的电容器元件试样。该电容器元件容量为13%±5% μF，元件中BOPP薄膜的厚度为6 μm，电极采用方块电阻为30 Ω/□的平板型锌铝合金电极。
1.2 老化试验方案
根据GB/T 17702—2021[11]，设置3种直流老化电场，分别为1.4En、1.5En和1.6En，其中En为金属化膜电容器的实际运行场强（235 kV/mm），另外设置一组不施加直流电场的电容器元件作为对照组。将4组试样放置在温度为60℃的鼓风控温箱中进行老化试验，每24 h取出试样测量电容量，以电容量下降5%为失效标准[12]，若该试样失效则停止老化试验。分别将对照组和经过1.4En、1.5En和1.6En直流电场老化后的电容器元件记为C0、C1、C2和C3。将对照组和老化失效后的电容器元件进行拆解获得BOPP薄膜，分别记为BOPP0、BOPP1、BOPP2和BOPP3。
1.3 测试方法
在老化过程中采用LCR测试仪（HIOKI 3532-50型）测试电容器元件的电容量，测试频率为50 Hz。电容量受测试温度影响，测试时采用红外测温仪测试元件温度以对电容量进行校准。
通过傅里叶变换红外光谱（FTIR，IR Prestige-21 Fourier型）和高温凝胶透色谱仪（HT-GPC，PL-GPC220）研究直流电场对BOPP薄膜分子链段结构的影响。FTIR测试采用透射模式，波数范围为4 000～400 cm-1。GPC测试是在150℃下将BOPP试样溶解于含有0.012 5%抗氧剂的1,2,4-三氯苯溶剂中进行，流速设置为1 mL/min。
通过X射线衍射仪（XRD，Bruker D8 ADVANCE A25型）和差示扫描量热仪（DSC，METTLER DSC822e型）分别研究老化前后BOPP薄膜试样晶型和结晶度的变化。XRD测试中，2θ范围为10°～30°。DSC测试中，温升范围为室温～200℃，升温速率为10℃/min。
通过动态热机械分析（DMA，METTLER SDTA861e型）研究BOPP薄膜试样非晶区分子链段的运动特性，温度范围为-40～60℃，升温速率为 3℃/min，测试频率为1、5、10、20 Hz，力为0.5 N，位移为30 μm。
在直流击穿试验中，采用直径为25 mm的球-球铜电极，为防止沿面闪络，将电极和BOPP薄膜试样均浸入硅油中进行试验，测试完毕后采用Weibull分布对数据进行统计分析。
2 试验结果
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2.1 电容器元件电容量衰减
电容器元件在老化试验过程中，电容量会不断下降，每24 h测得各个直流老化电场下电容量下降百分比（ΔC=(C0-C)/C0×100%，其中C0为初始电容量，C某时刻的电容量）随老化时间的变化曲线如图3所示。从图3可以看出，未施加电场的对照组电容量随时间几乎不变，而直流电场作用下的C1、C2、C3试样电容量均出现了下降，且电场越高，电容量下降速度越快。当电容器失效时，即电容量降为初始电容量的95%时，3组试样的寿命分别为955、525、263 h。在温度一定的条件下，施加电场E与固体绝缘的寿命L符合反幂定律（L=cE-n）[13]，这是IEC 61251推荐的典型电老化规律，其中c是常数，n是耐压系数，代表绝缘寿命随电压升高而降低的速度[14]。采用反幂定律对3组试样的寿命进行拟合，结果如图4所示。
值得注意的是，C1和C2试样的电容量下降速率随老化时间增加呈现先慢后快的趋势，出现了明显的“拐点”。相比于C2，C1容量下降缓慢阶段的持续时间较长，也就是说容量下降曲线的“拐点”出现时间较晚，大约在515 h左右，而C2的“拐点”出现在195 h左右。C3试样的电容量则随老化时间快速下降，没有明显“拐点”。由此可以看出，当老化电场较低时，电容量首先略有下降，而后快速下降，即从微小劣化逐渐累积转变成迅速失效，此外“拐点”出现时间和电容量下降速率很大程度上取决于施加的老化电场，当老化电场较高时，电容量呈现持续快速下降的规律，试样迅速失效。
2.2 BOPP薄膜微观特性
2.2.1 BOPP薄膜的分子链结构
为探究直流电场对电容器中BOPP薄膜分子链结构的影响，分别进行了FTIR和GPC试验，结果如图5和图6所示。图5中，3 000～2 800 cm-1处的透射峰对应于C-H的伸缩振动，1 500～1 350 cm-1处的透射峰对应于C-H的弯曲振动，而1 000～800 cm-1处的透射峰对应于等规聚丙烯的透射谱带[15]。从图5可以看到，经直流电场老化后BOPP薄膜的FTIR谱图的出峰位置和强度并未发生明显改变，说明老化过程中试样官能团未发生明显改变。
从图6可以看出，4种BOPP薄膜的重均分子量（Mw）分别为329 800、322 441、324 319和327 027。与对照组BOPP0相比，经直流电老化后BOPP1、BOPP2和BOPP3的Mw均有一定程度的降低，这表明直流电场会造成分子链断裂，且老化时间最长的BOPP1试样分子链断裂最为严重。有研究发现聚合物在高电压下长期运行会由于电子注入而发生断链[16]，并且当运行环境中有氧气参与时断链会更加严重[4]，虽然在本研究中分子链断裂现象并不是很明显，但仍表现出一定的趋势。
2.2.2 BOPP薄膜的结晶性能
聚丙烯厚片在双向拉伸的过程中会承受特定的热和力的作用，表面不稳定的β晶会向稳定的α晶转变，由于β晶的密度比α晶小，于是就形成了“环形山状”结晶[17]，这即是BOPP薄膜的粗化。为研究直流电场对BOPP结晶特性的影响，对老化前后的BOPP薄膜进行了XRD和DSC测试，结果分别如图7和图8所示。
从图7可以看出，4种BOPP薄膜没有出现β晶相，只呈现α晶，对应的特征峰出现在2θ为14.1°、16.8°以及18.6°处，分别对应于（110）、（040）、（130）晶面[18]。说明本研究中所使用的BOPP薄膜的β晶完全转变成α晶，并且直流电场的作用不能使试样的晶型发生变化。
结合图8，依据χc=ΔH/ΔH100×100%计算BOPP薄膜的结晶度，其中ΔH是试样的熔融焓，ΔH100是PP完全结晶时的熔融焓，其值为209 J/g[6]。计算得到BOPP薄膜的熔融温度（Tm）和结晶度（χc）如表1所示。从表1可以看出，4种BOPP薄膜的熔融温度均在170℃附近，对应于α结晶过程[18-19]。结晶度均在54%左右，老化后试样的结晶度变化量均未超过0.6%，表明电容器失效时BOPP薄膜的结晶度未发生改变。一般来说，分子链的排列很大程度上受热过程的影响[20]，在本研究中，老化温度固定为60℃且直流电场对电容器的温升影响很小，故BOPP薄膜的结晶特性没有明显改变。
2.2.3 BOPP薄膜的无定形区结构
一般来说，材料中结构松散的非晶区是首先发生劣化的区域。本研究对BOPP薄膜进行DMA测试研究非晶区的分子链段运动，4种BOPP薄膜在1、5、10、20 Hz的损耗模量E″谱图如图9所示。聚合物的弛豫峰对应于BOPP薄膜的玻璃化转变温度Tg，当温度低于Tg时，试样处于玻璃态，分子链被“冻结”，只能进行小幅振动，而当温度高于Tg时，试样由玻璃态转变为高弹态，分子链可进行长程运动。从图9可以看出，对照组BOPP0试样的Tg出现在9.1℃左右，经电场老化后各BOPP薄膜试样的Tg均有所降低，说明直流电场作用会降低分子链间的相互作用力。
为定量表征非晶区分子链段运动，对分子链段的运动活化能进行计算。一般而言，测试频率与材料Tg的关系符合式（1）所示阿伦尼乌斯方程[21]。
lnf=lnf0-ΔHRTg
式（1）中：f为Tg对应的频率；ΔH为分子链段运动活化能；f0为指前因子。
对图9中4种BOPP薄膜试样在不同频率下的Tg进行阿伦尼乌斯拟合，结果如图10所示。根据拟合直线计算得到BOPP0、BOPP1、BOPP2和BOPP3的分子链段运动活化能分别为5.62、3.94、4.20、5.47 eV。相比于对照组的BOPP0，经直流电场老化后的BOPP1、BOPP2和BOPP3活化能均有所降低，表明直流电场强使介质的分子链段运动势垒降低，使分子链段更容易运动。另外老化直流电场最低的BOPP1活化能最低，说明其性能劣化最为严重，这是由于C1电容器寿命最长，即BOPP1老化时间最长造成的。BOPP1、BOPP2和BOPP3的老化时长依次缩短，分子链段运动活化能依次升高，性能劣化程度依次降低。
2.3 BOPP薄膜的直流击穿特性
介质的微观结构与电气强度密切相关，对经直流电老化后BOPP薄膜试样的未击穿区域进行直流击穿试验，以表征薄膜的电气性能变化，试样剩余直流电气强度的Weibull分布及具体参数分别如图11和表2所示。从图11可以看出，4种BOPP薄膜试样剩余直流电气强度的Weibull分布均呈现出两段不同的趋势，M RITAMAKI等[5]和B GOSSE等[22]对聚丙烯薄膜的老化研究中发现其直流电气强度同样表现出类似的Weibull分布，表明出现了局部加速劣化。一般认为击穿概率为63.2%时对应的电气强度为特征电气强度，可以看到4种BOPP薄膜试样的特征电气强度呈现先下降后升高的趋势。对照组BOPP0的特征电气强度为555.7 kV/mm，经1.4En的直流电场作用后BOPP1的特征电气强度下降了5.52%，仅为525.0 kV/mm，随着老化场强的增加，BOPP2和BOPP3的特征电气强度分别为565.9 kV/mm和576.1 kV/mm，分别提高了1.84%和3.67%。在低击穿概率区，试样的电气强度呈现随老化电场的升高而升高的趋势，对照组的电气强度最低仅为270.1 kV/mm，而经1.6En的直流电场作用后BOPP3具有最高的电气强度，达339.7 kV/mm。
3 分析与讨论
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3.1 BOPP绝缘性能变化机理
聚合物的载流子传输特性与其分子排列密不可分，将根据图10获得的分子链段运动活化能与表2中不同击穿概率下的电气强度绘制于图12中。从图12可以看出，在高击穿概率区BOPP薄膜试样的电气强度对ΔH具有很强的依赖性，其中BOPP1试样的特征电气强度和分子链段运动活化能最低。BOPP薄膜是一种半结晶聚合物[2]，存在结晶区与非晶区，非晶区中存在未被分子完全占据的区域，这些由空位构成的区域称为低密度区、自由体积或空隙[23]。同时，BOPP中存在电弱点，与低密度区不同，电弱点来自于BOPP在生产和运行过程中引入的杂质、晶格缺陷等[24]。相比于结构紧凑的区域，电子在这低密度区或者电弱点区中更容易传输，并能获得足够的能量而导致击穿。
在非晶区，特别是低密度区，分子链段随机排布，链段运动活化能较低。在长时间的老化过程中，电应力的持续作用造成分子链断裂，会进一步削弱分子间的相互作用，促进分子位移并扩大自由体积，有利于电子的注入和传输，当电荷能量达到一定水平时，就会发生雪崩击穿。BOPP1的分子链断裂最为严重，因此分子链段相互作用力降低最明显，最终导致其特征电气强度最低。
特征电气强度主要受非晶区结构的影响，而局部区域的故障率主要由电弱点决定。当施加电压时，电弱点区域会发生击穿，电荷通过放电通道形成大电流，由于薄膜上的金属层厚度为纳米级，方阻很高，大电流产生的焦耳热会使击穿点附近的金属层蒸发并向外扩散，形成放电电弧，随后放电电弧熄灭，实现击穿点与电容器主体隔离，使电容器的绝缘性恢复，这一过程称之为“自愈”[25]。由于自愈特性，BOPP薄膜中的大部分弱点被击穿，即进行了“弱点清除”。老化电场越高会导致越多的弱点被清除，因此老化电场为1.6En的BOPP3具有最高的5%击穿概率对应的电气强度，为339.7 kV/mm，而完全没有经过弱点清除的BOPP0具有最低的5%击穿概率对应的电气强度，为270.1 kV/mm。此外薄膜经过1.4En、1.5En及1.6En的直流电场作用后，仍然存在低于老化场强的电气强度值，说明经过电老化后试样的电弱点不能被完全清除。
综上，老化后BOPP薄膜试样的电气强度可视为长期老化与短期弱点清除共同作用的结果，且有两种不同的原因使电容器失效，也就是说存在位于1.5En～1.6En的直流老化阈值电场，阈值电场作用下的电应力水平与薄膜绝缘水平相当。当老化电场低于阈值电场时，电应力水平低于薄膜绝缘水平，电容器可以在稳定状态下工作一段时间，但长期的老化作用会使介质薄膜的分子间相互作用减弱，即微小劣化逐渐累积，当劣化累积到一定程度时，介质的电弱点会加速产生随之引发自愈，电容器便进入迅速失效阶段，此时介质薄膜的直流击穿场强出现明显降低。当老化电场高于阈值电场时，电应力水平超过了薄膜绝缘水平，短期击穿占据主导地位，且介质薄膜的微观结构没有发生劣化，同时由于该老化条件下可以自愈清除的电弱点能量较大，介质薄膜的直流电气强度甚至略微有所升高。
3.2 电容器失效机理
电容器在直流老化的过程中，BOPP薄膜上的电弱点会不断产生，自愈也会不断发生，这意味着自愈清除面积不断增大。由于C=εS/d，其中C为电容量，ε为介质介电常数，S为极板面积，d为电极间距，可见电容量的损失值直接与自愈清除面积相关[26]。
BOPP在真空条件下发生的断链反应如图13所示[27]。从图13可以看出，直流电场作用造成BOPP分子断链的同时也会产生自由基，而自由基又会与分子链发生反应产生新的自由基，链式反应不断发生[16]。也就是说聚合物的劣化引发需要较长时间，而一旦劣化开始，降解速率就会不断加快。
从4组电容器的电容量下降曲线来看，C1和C2电容器的初始电容量下降速率较慢，这是由于此时电应力水平低于薄膜的绝缘水平，试样可稳定运行一段时间，在该阶段BOPP薄膜的性能未发生明显劣化，试样中原有的电弱点是导致自愈的主要原因。当老化时间达到“拐点”后，BOPP薄膜的性能开始劣化，并且随着老化的进行，劣化降解速率不断加快，导致新电弱点的产生速率也不断加快，相应地自愈击穿发生速率也逐渐加快，表现为电容器的电容量下降速率加快，即进入了加速降解阶段。前述试验结果表明C3电容器的介质性能劣化并不严重，说明C3电容器的电容量衰减是原始电弱点自愈导致的，BOPP薄膜的性能来不及劣化便已失效。这是因为施加在C3电容器上的电应力水平超过了薄膜的绝缘水平，载流子迁移势垒降低，使击穿更容易发生，表现为自愈不断发生，金属层面积持续损失，于是出现了电容量下降曲线近乎为直线的现象。
电容器的电容量随时间的衰减可以概括为如图14所示的两条曲线。曲线①表示老化电场低于阈值电场时的电容器电容量随时间的变化，其中I对应于由薄膜介质原有电弱点引发自愈而导致的电容量衰减阶段，II对应于薄膜介质加速劣化使电弱点加速产生引发自愈的加速衰减阶段，Ⅲ对应于电容器的失效；曲线②表示老化场强高于阈值场强时的电容器电容量随时间的变化，电容器原始电弱点不断进行自愈直至电容器失效。
4 结论
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本研究从设备和介质材料两个层面对超高直流电场作用下金属化膜电容器的老化特性进行了研究，主要得到以下结论：
（1）当老化温度一定时，超高直流电场（＞300 kV/mm）作用下的金属化膜电容器寿命遵循反幂定律。
（2）从电容器元件中拆解出来的BOPP薄膜测试结果显示，直流电老化会导致BOPP分子链断裂和分子链段运动活化能降低。
（3）电容器失效机理由阈值电场（位于1.5En～1.6En）所决定。当老化电场低于阈值电场时，电容器失效与BOPP薄膜性能的劣化密不可分；当老化电场高于阈值电场时，因薄膜原始电弱点自愈而发生的短期击穿是电容器失效的主要原因。
基金
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  • 国家自然科学基金资助项目(52107025)
  • 电网环境保护国家重点实验室开放基金资助项目(GYW51202101365)
文献
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2023年第56卷第5期
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doi: 10.16790/j.cnki.1009-9239.im.2023.05.009
  • 接收时间：2022-04-09
  • 首发时间：2025-11-21
  • 出版时间：2023-05-20
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  • 收稿日期：2022-04-09
  • 修回日期：2022-07-07
基金
国家自然科学基金资助项目(52107025)
电网环境保护国家重点实验室开放基金资助项目(GYW51202101365)
作者信息
    1西安交通大学 电力设备电气绝缘国家重点实验室,陕西 西安 710049
    2中国电力科学研究院有限公司 电网环境保护国家重点实验室,湖北 武汉 430074

通讯作者:

刘文凤（1982-），女（汉族），天津人，教授，主要从事先进介质材料的理论与应用研究。
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https://castjournals.cast.org.cn/joweb/jycl/CN/10.16790/j.cnki.1009-9239.im.2023.05.009
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2种不同金属材料的力学参数
科
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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