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Article(id=1203281565049663823, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1203281560800830004, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2025.05.009, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1719763200000, receivedDateStr=2024-07-01, revisedDate=1726156800000, revisedDateStr=2024-09-13, acceptedDate=null, acceptedDateStr=null, onlineDate=1764814280998, onlineDateStr=2025-12-04, pubDate=1747670400000, pubDateStr=2025-05-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1764814280998, onlineIssueDateStr=2025-12-04, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1764814280998, creator=13701087609, updateTime=1764814280998, updator=13701087609, issue=Issue{id=1203281560800830004, tenantId=1146029695717560320, journalId=1149653034449285133, year='2025', volume='58', issue='5', pageStart='1', pageEnd='144', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=0, articleOrder=1, issueType=-1, specialIssue=null, createTime=1764814279985, creator=13701087609, updateTime=1764814963861, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1203284429251784784, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1203281560800830004, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1203284429251784785, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1203281560800830004, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=63, endPage=72, ext={EN=ArticleExt(id=1203281565305516375, articleId=1203281565049663823, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Study on electrical performance of cellulose insulation paper modified by nano-TiO2 under electric-thermal coupling condition, columnId=1190369198472794288, journalTitle=Insulating Materials, columnName=Insulation Technology, runingTitle=null, highlight=

Cellulose insulation paper affects the reliability of transformer operation due to the long-term action of temperature and electric fields. The existing research mainly focuses on the modification effect of nano-particles on insulation paper under a single physical field, while the modification research under the combined effect of electric-thermal ageing is not yet perfect. This research prepared cellulose insulation papers modified by nano-TiO2 particle with mass fractions of 0, 1%, 3%, 5%, and 7%, and established corresponding molecular models based on molecular dynamics simulation. Combined with macroscopic electric-thermal combined ageing tests, the influence of electric field and temperature field on the electrical properties of modified cellulose insulation papers was studied, and the optimal modification content of nano-TiO2 was explored. The results show that the electrical properties of cellulose insulation paper are mainly affected by temperature, and the introduction of electric field accelerates the ageing of cellulose. After adding nano-TiO2 particles, the number of hydrogen bonds in the cellulose molecular model increases, the relative dielectric constant of the modified cellulose insulation paper decreases, and the electric strength increases. There is a threshold for the improvement of cellulose modification effect by the content of nano-TiO2, and the best modification effect on cellulose samples is achieved when the mass fraction of nano-TiO2 is 5%.

, articleAbstract=

Cellulose insulation paper affects the reliability of transformer operation due to the long-term action of temperature and electric fields. The existing research mainly focuses on the modification effect of nano-particles on insulation paper under a single physical field, while the modification research under the combined effect of electric-thermal ageing is not yet perfect. This research prepared cellulose insulation papers modified by nano-TiO2 particle with mass fractions of 0, 1%, 3%, 5%, and 7%, and established corresponding molecular models based on molecular dynamics simulation. Combined with macroscopic electric-thermal combined ageing tests, the influence of electric field and temperature field on the electrical properties of modified cellulose insulation papers was studied, and the optimal modification content of nano-TiO2 was explored. The results show that the electrical properties of cellulose insulation paper are mainly affected by temperature, and the introduction of electric field accelerates the ageing of cellulose. After adding nano-TiO2 particles, the number of hydrogen bonds in the cellulose molecular model increases, the relative dielectric constant of the modified cellulose insulation paper decreases, and the electric strength increases. There is a threshold for the improvement of cellulose modification effect by the content of nano-TiO2, and the best modification effect on cellulose samples is achieved when the mass fraction of nano-TiO2 is 5%.

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纤维素绝缘纸因长期受到温度场与电场的作用而影响变压器运行的可靠性。现有研究主要为针对单个物理场下纳米颗粒对绝缘纸改性效果的研究，而电-热联合老化作用下的改性研究尚未完善。本文制备了纳米TiO2颗粒质量分数分别为0、1%、3%、5%、7%的纳米TiO2改性纤维素绝缘纸，并根据分子动力学仿真模拟建立相应的分子模型，结合宏观电-热联合老化试验研究电场与温度场对改性纤维素绝缘纸电气性能的影响，探究纳米TiO2的最佳改性含量。结果表明：纤维素绝缘纸的电气性能主要受温度影响，电场的引入加速了纤维素的老化；添加纳米TiO2颗粒后，纤维素分子模型内的氢键数量增加，改性纤维素绝缘纸的相对介电常数降低，电气强度增大；纳米TiO2含量对纤维素改性效果的提升存在阈值，纳米TiO2的质量分数为5%时对纤维素样品的改性效果最佳。

, articleAbstract=

纤维素绝缘纸因长期受到温度场与电场的作用而影响变压器运行的可靠性。现有研究主要为针对单个物理场下纳米颗粒对绝缘纸改性效果的研究，而电-热联合老化作用下的改性研究尚未完善。本文制备了纳米TiO2颗粒质量分数分别为0、1%、3%、5%、7%的纳米TiO2改性纤维素绝缘纸，并根据分子动力学仿真模拟建立相应的分子模型，结合宏观电-热联合老化试验研究电场与温度场对改性纤维素绝缘纸电气性能的影响，探究纳米TiO2的最佳改性含量。结果表明：纤维素绝缘纸的电气性能主要受温度影响，电场的引入加速了纤维素的老化；添加纳米TiO2颗粒后，纤维素分子模型内的氢键数量增加，改性纤维素绝缘纸的相对介电常数降低，电气强度增大；纳米TiO2含量对纤维素改性效果的提升存在阈值，纳米TiO2的质量分数为5%时对纤维素样品的改性效果最佳。

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刘道生（1976-），男（汉族），江西赣州人，教授，主要从事电气绝缘、电力设备检测与故障诊断、变压器绝缘材料改性等方面的研究。
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崔车乐（2000-），男（汉族），广东茂名人，硕士生，主要从事变压器油纸绝缘材料与热老化的研究；

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崔车乐（2000-），男（汉族），广东茂名人，硕士生，主要从事变压器油纸绝缘材料与热老化的研究；

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崔车乐（2000-），男（汉族），广东茂名人，硕士生，主要从事变压器油纸绝缘材料与热老化的研究；

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journalId=1149653034449285133, articleId=1203281565049663823, language=EN, label=Table 1, caption=Young's modulus of each model GPa, figureFileSmall=null, figureFileBig=null, tableContent=
TiO2质量分数/%01357
303 K温度场13.4416.1217.3419.0218.22
电-温度场12.9415.6216.9018.8117.82
323 K温度场13.3315.8317.1018.8518.02
电-温度场12.6314.8516.5118.4117.53
343 K温度场12.7515.1916.8318.6717.82
电-温度场12.0514.6516.2118.2017.41
363 K温度场12.2914.8616.6818.3617.47
电-温度场11.5914.4915.7917.8816.94
383 K温度场11.7914.6016.0518.1917.09
电-温度场10.7113.8115.3517.7416.53
403 K温度场11.1613.9615.4617.4916.54
电-温度场10.3413.1214.7416.9715.95
423 K温度场10.3213.1614.7016.7615.83
电-温度场9.4712.2613.8616.2015.07
), ArticleFig(id=1203365328819561369, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1203281565049663823, language=CN, label=表1, caption=

各模型的杨氏模量

, figureFileSmall=null, figureFileBig=null, tableContent=
TiO2质量分数/%01357
303 K温度场13.4416.1217.3419.0218.22
电-温度场12.9415.6216.9018.8117.82
323 K温度场13.3315.8317.1018.8518.02
电-温度场12.6314.8516.5118.4117.53
343 K温度场12.7515.1916.8318.6717.82
电-温度场12.0514.6516.2118.2017.41
363 K温度场12.2914.8616.6818.3617.47
电-温度场11.5914.4915.7917.8816.94
383 K温度场11.7914.6016.0518.1917.09
电-温度场10.7113.8115.3517.7416.53
403 K温度场11.1613.9615.4617.4916.54
电-温度场10.3413.1214.7416.9715.95
423 K温度场10.3213.1614.7016.7615.83
电-温度场9.4712.2613.8616.2015.07
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电-热耦合条件下纳米TiO2改性纤维素绝缘纸的电气性能研究
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刘道生 1 , 崔车乐 1 , 陈欣 1 , 赖勇耀 2
绝缘材料 | 绝缘技术 2025,58(5): 63-72
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绝缘材料 | 绝缘技术 2025, 58(5): 63-72
电-热耦合条件下纳米TiO2改性纤维素绝缘纸的电气性能研究
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刘道生1, 崔车乐1, 陈欣1, 赖勇耀2
作者信息
  • 1.江西理工大学 电气工程与自动化学院，江西 赣州 341000
  • 2.国网江西赣州供电公司，江西 赣州 341001

    • 崔车乐（2000-），男（汉族），广东茂名人，硕士生，主要从事变压器油纸绝缘材料与热老化的研究；

通讯作者:

刘道生（1976-），男（汉族），江西赣州人，教授，主要从事电气绝缘、电力设备检测与故障诊断、变压器绝缘材料改性等方面的研究。
Study on electrical performance of cellulose insulation paper modified by nano-TiO2 under electric-thermal coupling condition
Daosheng LIU1, Chele CUI1, Xin CHEN1, Yongyao LAI2
Affiliations
  • 1. School of Electrical Engineering and Automation, Jiangxi University of Science and Technology, Ganzhou 341000, China
  • 2. State Grid Ganzhou Power Supply Company, Ganzhou 341001, China
出版时间: 2025-05-20 doi: 10.16790/j.cnki.1009-9239.im.2025.05.009
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摘要
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纤维素绝缘纸因长期受到温度场与电场的作用而影响变压器运行的可靠性。现有研究主要为针对单个物理场下纳米颗粒对绝缘纸改性效果的研究，而电-热联合老化作用下的改性研究尚未完善。本文制备了纳米TiO2颗粒质量分数分别为0、1%、3%、5%、7%的纳米TiO2改性纤维素绝缘纸，并根据分子动力学仿真模拟建立相应的分子模型，结合宏观电-热联合老化试验研究电场与温度场对改性纤维素绝缘纸电气性能的影响，探究纳米TiO2的最佳改性含量。结果表明：纤维素绝缘纸的电气性能主要受温度影响，电场的引入加速了纤维素的老化；添加纳米TiO2颗粒后，纤维素分子模型内的氢键数量增加，改性纤维素绝缘纸的相对介电常数降低，电气强度增大；纳米TiO2含量对纤维素改性效果的提升存在阈值，纳米TiO2的质量分数为5%时对纤维素样品的改性效果最佳。

电-热耦合  /  老化试验  /  分子模拟  /  电气性能

Cellulose insulation paper affects the reliability of transformer operation due to the long-term action of temperature and electric fields. The existing research mainly focuses on the modification effect of nano-particles on insulation paper under a single physical field, while the modification research under the combined effect of electric-thermal ageing is not yet perfect. This research prepared cellulose insulation papers modified by nano-TiO2 particle with mass fractions of 0, 1%, 3%, 5%, and 7%, and established corresponding molecular models based on molecular dynamics simulation. Combined with macroscopic electric-thermal combined ageing tests, the influence of electric field and temperature field on the electrical properties of modified cellulose insulation papers was studied, and the optimal modification content of nano-TiO2 was explored. The results show that the electrical properties of cellulose insulation paper are mainly affected by temperature, and the introduction of electric field accelerates the ageing of cellulose. After adding nano-TiO2 particles, the number of hydrogen bonds in the cellulose molecular model increases, the relative dielectric constant of the modified cellulose insulation paper decreases, and the electric strength increases. There is a threshold for the improvement of cellulose modification effect by the content of nano-TiO2, and the best modification effect on cellulose samples is achieved when the mass fraction of nano-TiO2 is 5%.

electric-thermal coupling  /  ageing test  /  molecular simulation  /  electrical performance
刘道生, 崔车乐, 陈欣, 赖勇耀. 电-热耦合条件下纳米TiO2改性纤维素绝缘纸的电气性能研究. 绝缘材料, 2025 , 58 (5) : 63 -72 . DOI: 10.16790/j.cnki.1009-9239.im.2025.05.009
Daosheng LIU, Chele CUI, Xin CHEN, Yongyao LAI. Study on electrical performance of cellulose insulation paper modified by nano-TiO2 under electric-thermal coupling condition[J]. Insulating Materials, 2025 , 58 (5) : 63 -72 . DOI: 10.16790/j.cnki.1009-9239.im.2025.05.009
正文
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0 引言
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油浸式变压器是我国电力系统中的核心设备[1-4]。变压器绝缘油、纸板等构成的油-纸复合绝缘结构承担着油浸式变压器的电气绝缘任务[5-6]。油浸式变压器油-纸绝缘系统长期受电场、温度场环境变化的影响，其电气性能逐渐降低[7-10]，进而引发绝缘故障。相比于绝缘油，绝缘纸电气性能的带电检测手段较少，若绝缘纸发生故障，更换难度非常大，且绝缘纸的质量和寿命将直接影响油浸式变压器的使用年限[11]。为提高油浸式变压器的可靠性，保证电力系统的稳定运行，提高绝缘纸的电气性能至关重要。
利用纳米材料对绝缘纸进行改性以提高纤维素绝缘纸的电气性能已成为当下研究热点之一。目前，纳米改性技术在各个领域都有许多成熟研究。陈庆国等[12]探究了添加纳米SiC对绝缘纸板介电性能的影响。廖瑞金等[13-15]研究了纳米Al2O3、纳米TiO2等纳米材料对绝缘纸电气性能的影响，并开展了一系列加速老化试验和仿真试验。结果表明纳米Al2O3、TiO2的添加改变了绝缘纸表面微观结构，使纤维素分子间的陷阱能级分布发生改变，通过添加适量的纳米材料，绝缘纸的电气性能会得到一定程度的提高。
分子模拟技术能够从微观角度揭示材料之间的相互作用机理，在绝缘材料领域的研究中被广泛应用[16-19]。王有元等[20-21]通过分子动力学模拟研究了变压器运行过程中的温度、电场、水分以及酸对绝缘纸性能的影响，为探索绝缘纸老化机理提供了重要的理论依据。张松等[22]在试验中测试了纳米Al2O3对绝缘纸改性的效果，并运用分子动力学模拟对改性绝缘纸的微观参数进行研究。试验和模拟结果均表明，纳米Al2O3的添加提升了绝缘纸的热稳定性。
然而，现有的纤维素绝缘纸改性研究大多集中在常规状态下纳米材料对纤维素纸的改性效果，而在电-热耦合条件下对纤维素纸的改性研究鲜有报道。本文搭建电-热联合加速老化试验平台，对不同质量分数（0、1%、3%、5%、7%）纳米TiO2改性纤维素绝缘纸开展电-热联合加速老化试验；建立不同含量纳米TiO2改性纤维素分子模型，分别在温度场与电场-温度场下对其进行分子动力学模拟。从宏观与微观两个方面分析电-热耦合条件下纤维素绝缘纸电气性能的变化规律，研究电场与温度场对纤维素绝缘纸电气性能的影响机理，得到改性效果最佳的纳米TiO2/纤维素复合材料。
1 试验
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1.1 原材料
ZL-PB型纤维素原浆纸板，南通中菱电力科技股份有限公司；纳米TiO2，粒径为10 nm，南京海泰纳米材料有限公司；克拉玛依25#变压器油，美央环保科技（上海）有限公司。
1.2 样品制备
纤维素绝缘纸板经过打浆、过滤和解离等过程后与纳米TiO2粒子悬浊液共混可以制得纳米改性纤维素纸板。为了不引入离子等杂质，实验室改性纤维素纸板的整个制备过程均使用电导率为10 μS/cm的去离子水，将不同质量经硅烷偶联剂KH-550表面改性的纳米TiO2分别与去离子水混合，制成纳米粒子悬浊液，之后以5 000 r/min的转速搅拌30 min；随后将不同纳米粒子悬浊液分别与纤维素纸浆共混，再装入解离器中以 300 r/min的转速搅拌10 min，使纤维素与纳米TiO2混合均匀；最后使用山东安尼麦特仪器有限公司生产的AT-CZ-1型纸页成型器对改性纤维素纸浆进行抄造，经过干燥、压光制备得到纳米TiO2质量分数分别为0、1%、3%、5%、7%的改性绝缘纸板，样品分别命名为X%TiO2/纤维素纸板，X%为纳米TiO2的质量分数。在不含纳米粒子的绝缘纸板制备过程中，多次（6次以上）测量其质量损失，得到纤维素质量损失率约为5.0%。加入纳米粒子后，改性纤维素纸板中的纤维素质量损失率仍约为5.0%，说明实际改性绝缘纸板中的纳米TiO2质量分数仍为1%、3%、5%、7%。如果纤维素质量损失率偏差过大，需要重复造纸，待其质量损失率合格后，方能采用其制备样品。改性纤维素纸板的制备流程如图1所示。
1.3 电-热联合加速老化处理
将制得的改性纤维素纸板样品放在85℃的真空干燥箱中干燥48 h以除去水分，并对25#变压器油进行过滤和干燥。为模拟绝缘纸样品在温度场和电场联合作用下的老化环境，本文设计并搭建了电-热联合加速老化试验平台，如图2所示。该平台加速电老化模块采用板-板结构试验电极，上、下电极均是直径为75 mm的等径黄铜极板。加速电老化的电压设定为3.5 kV（工频），整个电老化装置浸入25#变压器油中，再将油箱放置在温度为130℃的老化室内，以加速热老化。本文对纳米TiO2含量为0、1%、3%、5%、7%的纤维素纸板样品进行了电-热老化联合试验，每组为期10天。在试验的第0天、第1天、第3天、第5天和第10天对样品进行性能测试。
1.4 相对介电常数测试
介电常数是衡量绝缘材料电气性能的宏观参数，其反映了绝缘材料在静电场作用下的极化性质。在变压器运行过程中，绝缘纸介电常数的变化会影响变压器内部的电场分布，容易引发击穿或闪络等故障，因此研究绝缘纸运行过程中的介电常数变化规律非常重要。本文搭建了三电极相对介电常数测量系统（如图3所示），分别对老化时间为0、1、3、5、10天的不同含量纳米TiO2改性纤维素样品进行相对介电常数测量。
该测试系统由高压介质损耗测试仪、三电极系统和温控箱等组成，其中高压线和高压电极相连，屏蔽线和保护电极相连，测试电极通过芯线与测试仪器的样品输入端相连。三电极系统相较于两电极系统多了一个保护电极，测量样品电容时，保护电极会吸收边缘电场，从而去除边缘电容对测量结果产生的影响。本文使用武汉德威电力测试设备有限公司生产的GWS-4C型高压介质损耗测试仪，采用正接法测量样品在工频下的电容，并通过式（1）计算样品的相对介电常数[23]。
εr=C⋅dε0⋅S
式（1）中：C为样品的电容，F；ε0为真空介电常数，取值为8.854×10-12 F/m；S为电容极板面积，m2；d为极板间距，m。
1.5 击穿测试
本文对老化时间分别为0、1、3、5、10天的不同含量纳米TiO2改性纤维素样品进行交流击穿测试，测试电极装置如图4所示。该电极装置由直径为25 mm的上部电极和直径为75 mm的下部电极组成。测试变压器的容量为50 kVA，升压速度设置为500 V/s，通过测量样品的交流击穿电压，进而计算电气强度。
试验具体步骤如下：首先将改性纤维素纸板样品和25#变压器油分别放入真空干燥箱中进行干燥；然后将干燥后的样品放置在两电极轴中心处，连接好设备后将测试电极装置放入油罐中，确保绝缘纸样品浸没于25#变压器油中；最后逐步对绝缘纸样品进行升压测试，10～20 s内未击穿再继续升压，升压速率为500 V/s，直到击穿为止，记录此时的击穿电压。重复实验3～5次，取平均值作为测试结果。
2 结果与分析
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2.1 样品基本表征
通过扫描电子显微镜（SEM，Hitachi Regulus8100型）观测了不同纳米TiO2含量纤维素纸板的表面形貌，结果如图5所示。由图5可知，纯纤维素纸板表面存在许多空穴和纤维素断裂现象，而5%TiO2/纤维素纸板具有紧密的纤维排列和相对光滑的表面，纤维素断裂现象比其他样品少，说明纳米TiO2的加入使纤维素的孔隙变小，且均有更高的均匀性。但当纳米TiO2质量分数增加到7%时，纳米粒子团聚现象严重，改性纤维素绝缘纸板表面粗糙。
采用能量色散谱仪（EDS，Excite+型）检测纯纤维素样品和不同纳米TiO2含量改性纤维素样品表面区域的元素，结果如图6所示。从图6可以看出，与其他纳米粒子改性样品相比，5%TiO2/纤维素纸板表面的氧元素含量最低，这主要是因为纳米TiO2与水反应形成许多羟基，羟基又与纤维素紧密结合，从而减少了纤维素表面的TiO2，提高了纤维素的表面平整度。然而，过量添加纳米粒子会增加氧元素的含量，进而增强纳米TiO2和纤维素基质之间的静电力，导致大量纳米粒子聚集，影响样品的表面形态，如图5(e)中SEM图所示。
2.2 相对介电常数变化规律分析
不同纳米TiO2含量改性绝缘纸样品的相对介电常数测试结果如图7所示。从图7可知，改性绝缘纸样品的相对介电常数随着老化的进行逐渐增大。在老化中后期，纯纤维素纸样品的相对介电常数明显高于改性绝缘纸样品，其中5%TiO2/纤维素绝缘纸样品的相对介电常数最低，在老化第0天与老化第10天时分别为2.84与3.37。
绝缘纸老化伴随着纤维素分子链的裂解，纤维素分子之间的相互作用力减弱，其极性基团也会因缺少束缚变得更容易极化，因此相对介电常数会随着老化的进行逐渐增大。纳米TiO2与纤维素之间因形成氢键而紧密连接，抑制了纤维素中羟基等极性基团的极化[24]，使改性纤维素绝缘纸样品的相对介电常数低于纯纤维素绝缘纸。但随着纳米颗粒含量的增加，纳米TiO2出现团聚现象，分子间氢键数量减少，而极性基团缺少束缚更容易发生极化，因此7%TiO2/纤维素绝缘纸样品的相对介电常数大于5%TiO2/纤维素绝缘纸样品。
2.3 电气强度变化规律分析
不同纳米TiO2含量改性绝缘纸样品的电气强度测试结果如图8所示。由图8可知，在老化初期，绝缘纸的绝缘性能良好且受温度场和电场的影响较小，其内部纤维素分子链的裂解速度较为缓慢，电气强度下降速度也较为缓慢。随着电-热联合老化时间的增加，温度的长期影响使纤维素的热降解活动加剧，造成主链断裂和侧基从主链上脱去[25]；电场则增强了纤维素的极化，进而加速绝缘纸纤维素结构的破坏。两种因素的叠加使电-热联合老化后期的绝缘纸劣化过程显著加剧，因此绝缘纸的工频交流电气强度陡然下降。
从图8还可以看出，改性纤维素绝缘纸样品的电气强度均高于纯纤维素绝缘纸。随着纳米TiO2质量分数的增加，改性纤维素绝缘纸样品的电气强度逐渐提高。在不同老化阶段，5%TiO2/纤维素绝缘纸样品的工频交流电气强度始终最高，在老化第0天与老化第10天时分别为29.43 kV/mm与14.23 kV/mm。而过量的纳米TiO2粒子会发生团聚，破坏界面层结构，分子间作用力减弱，因此7%TiO2/纤维素绝缘纸样品的电气强度小于5%TiO2/纤维素样品。
3 分子动力学模拟
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3.1 模型构建与优化
本文基于D N THEODOROU等[26]提出的静态退火法进行模型构建，以40条聚合度为10的纤维素分子链与纳米TiO2粒子构建纳米TiO2质量分数分别为0、1%、3%、5%、7%的改性纤维素分子模型，5种模型的分子结构如图9所示。其中纳米TiO2团簇半径为5Å，其分子结构如图9(f)所示。模型的目标密度设为1.5 g/cm3。
在进行分子动力学计算前，首先对建立的每个模型进行20 000步的结构优化和能量最小化处理。为了消除模型内部残余应力和松弛分子链结构，在模型能量最小化和结构优化的基础上对模型进行从300 K到500 K的退火处理，循环5次，温度间隔为50 K，每个间隔下的计算时长为1 000 fs，系综为NVT（固定粒子数、固定体积、固定温度）。退火后，提取模型处理后能量最小的结构构象进行分子动力学弛豫，使得模型的性能接近真实材料性能。随后对模型依次进行NVT与NPT（固定粒子数、固定压强、固定温度）分子动力学模拟。
3.2 氢键数量分析
氢键可以表示为“X－H…Y”，其中X和Y一般为电负性较大的元素，X称为施主，Y称为受主，且Y原子有一对或一对以上的孤对电子，X－H称为质子供体。在本文构造的纳米TiO2改性纤维素绝缘纸分子模型中，形成氢键的原子仅为H原子与O原子，故氢键类型全为O－H…O。本文氢键的形成条件为：氢原子和受主之间的距离小于2Å，施主、氢原子和受主之间形成的角大于110°。纤维素材料内存有大量氢键，其对纤维素热稳定性的影响甚至超过了纤维素内化学键的作用。本文通过自编脚本计算5组模型在303～423 K下的氢键数量，取平均值作为最终结果，每40 K提取一次数据。5组模型的平均氢键数量变化规律如图10所示。
从图10可以看出，随着温度的升高，纤维素分子活动加剧，部分氢键被破坏，5组模型的氢键数量均随着温度的升高而减少。在相同温度下，改性纤维素模型的平均氢键数量均高于纯纤维素模型，其中5%TiO2/纤维素模型的氢键数量最多。在热老化条件下，303 K时纯纤维素模型的氢键数量为1 831，在423 K时降至1 622；303 K时5%TiO2/纤维素模型的氢键数量为2 203，在423 K时降至2 050。说明加入纳米TiO2粒子后，纤维素分子链与纳米粒子形成了强烈的界面作用，不仅增加了氢键的数量，还有效地抑制了氢键的断裂。在纳米TiO2质量分数达到7%时，粒子发生团聚，破坏了原本的稳定结构，导致氢键数量减少，纤维素分子间相互作用力减弱。
从图10还可以看出，电场的引入不仅使纤维素分子链受到电场的极化作用，导致分子链的排列发生变化，使原本稳定的结构被破坏，纤维素分子链间的氢键数量减少，还加剧了氢键数量随温度升高而下降的趋势，温度越高，电场对模型氢键数量的影响越大。
3.3 相对介电常数分析
在油-纸绝缘结构中，较低的介电常数有利于延缓电老化的发展进程。本文根据M NEUMANN[27]提出的偶极矩法来计算纤维素模型在模拟过程中的相对介电常数（ε），具体计算公式如式（2）所示。
ε=1+13ε0kBTVM2-M2
式（2）中：M为模拟中每一帧分子的偶极矩；〈…〉为体系的平均值；V为模型的体积，m3；T为热力学温度，K；kB为玻尔兹曼常数；ε0为真空介电常数，取值为8.854×10-12 F/m。
对5组模型分别在温度场与电-温度场下进行NPT分子动力学模拟，温度范围设置为303～423 K，记录5组模型的偶极矩波动，根据式（2）计算模型的相对介电常数，结果如图11所示。从图11可以看出，随着温度升高，5组模型的相对介电常数均呈现先增大后减小的变化趋势。这是因为一开始随着温度升高，纤维素分子链的热运动加剧，氢键数量开始减少，分子极化作用增强，模型的相对介电常数增大；在温度达到383 K后，纤维素分子链的运动程度进一步增强，偶极子发生解取向作用，这种解取向作用抑制了纤维素分子的极化作用，导致模型的相对介电常数减小。引入电场后，纯纤维素模型的相对介电常数增大，且温度越高，相对介电常数的增幅也越大。观察4组改性纤维素模型，也存在类似的趋势。
从图11还可以看出，改性纤维素模型的相对介电常数均比纯纤维素模型的要小。这主要是因为添加TiO2颗粒后，TiO2与纤维素形成界面效应，界面层的介电常数主导着材料的介电性能。由于界面层的介电常数较小，复合体系的总体介电常数较小。同时，TiO2颗粒的加入增加了氢键的数量，使得界面区域中的高分子链段或侧基不易转向，导致分子极化作用减弱。随着TiO2含量的增加，界面层的氢键数量增加，相对介电常数继续减小。在本次实验中，5%TiO2/纤维素模型的相对介电常数最低。在温度场条件下，303 K时纯纤维素模型的相对介电常数为2.911，5%TiO2/纤维素模型的相对介电常数为2.418，相比纯纤维素模型降低了16.9%；在纳米TiO2质量分数达到7%时，由于粒子发生团聚，破坏了界面层结构，氢键数量减少，模型的相对介电常数相对于5%TiO2/纤维素模型增大。
3.4 电气强度分析
为了验证宏观电-热联合老化试验中电气强度的测试结果，本文对5组模型的电气强度进行了计算。材料的电气强度与样品的厚度遵循反幂定律[28]，由于分子模型与纤维素纸板厚度差距太大，模拟得到的电气强度与试验测得的电气强度差距较大，但并不影响趋势分析。电气强度的计算公式如式（3）所示[29]。
Eb=0.6(Yε0εr)12
式（3）中：Eb为电气强度，kV/m；Y为杨氏模量，GPa；ε0为真空介电常数，取值为8.854×10-12 F/m；εr为模型的相对介电常数。
对5组模型分别在温度场与电-温度场下进行NPT分子动力学模拟，通过Constant strain法计算模型的杨氏模量，每隔20 K记录一次数据，得到5组模型在温度场与电-温度耦合场下杨氏模量的变化，如表1所示。根据式（3）计算5组模型的电气强度，结果如图12所示。
从图12可以看出，热老化条件下，所有模型的电气强度均随着温度升高而降低，纯纤维素模型的电气强度在303 K时为433.3 kV/m，在423 K时下降至360.1 kV/m；引入电场后，纯纤维素模型的电气强度在303 K时为407.4 kV/m，在423 K时下降至329.0 kV/m。电场的引入导致模型中电离粒子的数量增加，电流迅速增大，局部电场更易畸变，因此模型的电气强度下降。
从图12还可以看出，同一温度下，改性纤维素模型的电气强度均高于纯纤维素模型。说明添加TiO2颗粒后，体系内的界面相互作用增强，氢键数量增加，分子链的热运动被抑制，电子的动能减弱，不易发生碰撞电离，电场不易发生畸变，进而提升了纤维素绝缘纸的电气强度。随着TiO2含量增加，模型的电气强度呈现先增大后减小的变化趋势，其中5%TiO2/纤维素模型的电气强度最大。在热老化条件下，303 K时5%TiO2/纤维素模型的电气强度为565.5 kV/m，相比纯纤维素模型提升了30.5%，在423 K时电气强度下降至503.9 kV/m，相比纯纤维素模型提升了39.9%。当TiO2含量达到阈值时，纳米粒子出现团聚，界面区域产生重叠，体系内部的陷阱增加，局部电场畸变率增大，导致模型的电气强度降低，因此7%TiO2/纤维素模型的电气强度比5%TiO2/纤维素模型低。
4 结论
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（1）添加纳米TiO2颗粒能增加纤维素分子间氢键的数量，提高分子间的相互作用力，削弱分子的极化作用，有效提高了纤维素绝缘纸的介电性能与电气强度。
（2）纳米TiO2颗粒对纤维素绝缘纸性能的提升效果存在阈值，5%TiO2对纤维素的改性效果最佳，因此纳米TiO2的最佳质量分数为5%。
（3）纤维素绝缘纸的电气性能主要受温度影响，电场的引入会增强分子的极化作用，减少分子间的氢键数量，降低分子间的相互作用力，从而加速纤维素的劣化。
基金
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  • 国家自然科学基金资助项目(52167017)
  • 江西省自然科学基金资助项目(20224BAB204054)
  • 赣鄱俊才支持计划-主要学科学术和技术带头人培养项目(20232BCJ22006)
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2025年第58卷第5期
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doi: 10.16790/j.cnki.1009-9239.im.2025.05.009
  • 接收时间：2024-07-01
  • 首发时间：2025-12-04
  • 出版时间：2025-05-20
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  • 收稿日期：2024-07-01
  • 修回日期：2024-09-13
基金
国家自然科学基金资助项目(52167017)
江西省自然科学基金资助项目(20224BAB204054)
赣鄱俊才支持计划-主要学科学术和技术带头人培养项目(20232BCJ22006)
作者信息
    1.江西理工大学 电气工程与自动化学院，江西 赣州 341000
    2.国网江西赣州供电公司，江西 赣州 341001

通讯作者:

刘道生（1976-），男（汉族），江西赣州人，教授，主要从事电气绝缘、电力设备检测与故障诊断、变压器绝缘材料改性等方面的研究。
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https://castjournals.cast.org.cn/joweb/jycl/CN/10.16790/j.cnki.1009-9239.im.2025.05.009
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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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