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Article(id=1222482902261158251, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1222482900604408161, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2021.03.006, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1587830400000, receivedDateStr=2020-04-26, revisedDate=1591632000000, revisedDateStr=2020-06-09, acceptedDate=null, acceptedDateStr=null, onlineDate=1769392236533, onlineDateStr=2026-01-26, pubDate=1613750400000, pubDateStr=2021-02-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1769392236533, onlineIssueDateStr=2026-01-26, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1769392236533, creator=13041195026, updateTime=1769392236533, updator=13041195026, issue=Issue{id=1222482900604408161, tenantId=1146029695717560320, journalId=1149653034449285133, year='2021', volume='54', issue='3', pageStart='1', pageEnd='107', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1769392236137, creator=13041195026, updateTime=1770971768252, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1229107938527342697, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1222482900604408161, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1229107938527342698, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1222482900604408161, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=36, endPage=41, ext={EN=ArticleExt(id=1222482902571536756, articleId=1222482902261158251, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Effects of Electric Field and Temperature Synergism on Diffusion Behavior of Water Molecules in Nano-SiO2 Modified Insulating Oil, columnId=1190369066675179686, journalTitle=Insulating Materials, columnName=Material Research, runingTitle=null, highlight=null, articleAbstract=

The effects of electric field and temperature on the diffusion behavior of water molecules in nano-SiO2 modified insulating oil were studied by molecular simulation technology. The results show that the water molecules are polarized under electric field, and the water molecules would change from an original disordered arrangement to an ordered arrangement along the direction of electric field. Therefore, under the action of electric field, the Brownian motion of water molecules weakens, and the diffusion ability of water molecules in oil decreases. The electrostatic force between water molecules and oil medium was enhanced by electric field, which is 2‒3 times bigger than that without electric field. This is also the main reason for the increase of interaction energy between water molecules and oil medium under electric field. In addition, under the action of electric field, the free volume fraction of the model decreases, and the effect of temperature on the hydrogen bond between O and H atoms in the model weakens.

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利用分子模拟技术研究了电场和温度对纳米SiO2改性绝缘油中水分子扩散行为的影响。结果表明：电场会使水分子发生极化，使得水分子由原本的无序排列变为沿着电场方向的有序排列。因此，电场的加入减弱了水分子的布朗运动，降低了水分子在油中的扩散能力；而且电场的加入增强了水分子与油介质之间的静电作用力，其数值是无电场作用下的2～3倍，这也是电场作用下两者间相互作用能增大的主要原因。此外，在电场的作用下，模型的自由体积分数减小，温度对模型中O原子和H原子之间氢键的影响减弱。

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邱秦攀（1996-），男（汉族），重庆人，硕士生，研究方向为绝缘电介质材料老化与改性；

唐超（1981-），男（汉族），四川自贡人，教授，主要从事高电压绝缘技术的研究。

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邱秦攀（1996-），男（汉族），重庆人，硕士生，研究方向为绝缘电介质材料老化与改性；

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邱秦攀（1996-），男（汉族），重庆人，硕士生，研究方向为绝缘电介质材料老化与改性；

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唐超（1981-），男（汉族），四川自贡人，教授，主要从事高电压绝缘技术的研究。

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唐超（1981-），男（汉族），四川自贡人，教授，主要从事高电压绝缘技术的研究。

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成分链烃环烷烃合计
一环二环三环四环
质量分数/%11.615.528.523.39.788.6
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环烷基矿物油的成分组成

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成分链烃环烷烃合计
一环二环三环四环
质量分数/%11.615.528.523.39.788.6
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项目303 K323 K343 K363 K383 K
FFV/%0.009 70.009 90.010 10.010 30.010 5
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加电场时模型的自由体积分数

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FFV/%0.009 70.009 90.010 10.010 30.010 5
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项目303 K323 K343 K363 K383 K
FFV/%0.068 280.068 30.069 360.070 430.072 54
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未加电场时模型的自由体积分数

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项目303 K323 K343 K363 K383 K
FFV/%0.068 280.068 30.069 360.070 430.072 54
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项目303 K323 K343 K363 K383 K
Etotal-48.57-47.89-44.33-42.95-41.675
Evdw-42.56-40.484-37.863-37.21-35.759
Eelec-4.86-5.273-5.3165-4.588-4.7655
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电场作用下水分子和油分子间的相互作用能

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项目303 K323 K343 K363 K383 K
Etotal-48.57-47.89-44.33-42.95-41.675
Evdw-42.56-40.484-37.863-37.21-35.759
Eelec-4.86-5.273-5.3165-4.588-4.7655
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项目303 K323 K343 K363 K383 K
Etotal-43.907-42.845-41.922-40.895-39.714
Evdw-41.66-40.685-39.12-38.05-36.94
Eelec-1.79-1.79-1.81-1.742-1.73
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无电场作用下水分子和油分子间的相互作用能

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项目303 K323 K343 K363 K383 K
Etotal-43.907-42.845-41.922-40.895-39.714
Evdw-41.66-40.685-39.12-38.05-36.94
Eelec-1.79-1.79-1.81-1.742-1.73
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电场和温度协同作用对纳米SiO2改性绝缘油中水分子扩散行为的影响
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邱秦攀 1 , 张静文 1 , 王谦 2 , 刘熊 2 , 田汶鑫 1 , 唐超 1
绝缘材料 | 材料研究 2021,54(3): 36-41
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绝缘材料 | 材料研究 2021, 54(3): 36-41
电场和温度协同作用对纳米SiO2改性绝缘油中水分子扩散行为的影响
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邱秦攀1, 张静文1, 王谦2, 刘熊2, 田汶鑫1, 唐超1
作者信息
  • 1西南大学 工程技术学院，重庆 400715
  • 2国网重庆市电力公司电力科学研究院，重庆 401123

    • 邱秦攀（1996-），男（汉族），重庆人，硕士生，研究方向为绝缘电介质材料老化与改性；

    唐超（1981-），男（汉族），四川自贡人，教授，主要从事高电压绝缘技术的研究。

Effects of Electric Field and Temperature Synergism on Diffusion Behavior of Water Molecules in Nano-SiO2 Modified Insulating Oil
Qinpan QIU1, Jingwen ZHANG1, Qian WANG2, Xiong LIU2, Wenxin TIAN1, Chao TANG1
Affiliations
  • 1College of Engineering and Technology, Southwest University, Chongqing 400715, China
  • 2Electric Power Research Institute of State Grid Chongqing Electric Power Company, Chongqing 401123, China
出版时间: 2021-02-20 doi: 10.16790/j.cnki.1009-9239.im.2021.03.006
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摘要
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利用分子模拟技术研究了电场和温度对纳米SiO2改性绝缘油中水分子扩散行为的影响。结果表明：电场会使水分子发生极化，使得水分子由原本的无序排列变为沿着电场方向的有序排列。因此，电场的加入减弱了水分子的布朗运动，降低了水分子在油中的扩散能力；而且电场的加入增强了水分子与油介质之间的静电作用力，其数值是无电场作用下的2～3倍，这也是电场作用下两者间相互作用能增大的主要原因。此外，在电场的作用下，模型的自由体积分数减小，温度对模型中O原子和H原子之间氢键的影响减弱。

绝缘油  /  纳米粒子  /  分子模拟  /  相互作用能  /  自由体积

The effects of electric field and temperature on the diffusion behavior of water molecules in nano-SiO2 modified insulating oil were studied by molecular simulation technology. The results show that the water molecules are polarized under electric field, and the water molecules would change from an original disordered arrangement to an ordered arrangement along the direction of electric field. Therefore, under the action of electric field, the Brownian motion of water molecules weakens, and the diffusion ability of water molecules in oil decreases. The electrostatic force between water molecules and oil medium was enhanced by electric field, which is 2‒3 times bigger than that without electric field. This is also the main reason for the increase of interaction energy between water molecules and oil medium under electric field. In addition, under the action of electric field, the free volume fraction of the model decreases, and the effect of temperature on the hydrogen bond between O and H atoms in the model weakens.

insulating oil  /  nanoparticles  /  molecular simulation  /  interaction energy  /  free volume
邱秦攀, 张静文, 王谦, 刘熊, 田汶鑫, 唐超. 电场和温度协同作用对纳米SiO2改性绝缘油中水分子扩散行为的影响. 绝缘材料, 2021 , 54 (3) : 36 -41 . DOI: 10.16790/j.cnki.1009-9239.im.2021.03.006
Qinpan QIU, Jingwen ZHANG, Qian WANG, Xiong LIU, Wenxin TIAN, Chao TANG. Effects of Electric Field and Temperature Synergism on Diffusion Behavior of Water Molecules in Nano-SiO2 Modified Insulating Oil[J]. Insulating Materials, 2021 , 54 (3) : 36 -41 . DOI: 10.16790/j.cnki.1009-9239.im.2021.03.006
正文
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0 引言
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油纸绝缘是变压器的主要绝缘系统，一旦其发生故障，会影响变压器的运行安全。在变压器运行中，油纸在电场、温度、机械振动等应力的综合作用下会逐渐老化，使得变压器中的水分含量随着运行时间的延长而逐渐增加[1-2]。水分会降低油纸绝缘系统的电气和力学性能[3-7]，且水分的积累会加速油纸绝缘系统的老化[8-10]。
水分子在绝缘油中的扩散行为除了受温度影响外，也会受到变压器中电场的影响[11-13]。其中电场作为一个重要的外界因素，对于油纸绝缘系统的老化起着至关重要的作用。在实际的变压器运行过程中，水分受电场的影响会发生迁移，从而降低绝缘油的局部放电起始电压，增加油纸界面的导电粒子，使绝缘系统遭到破坏。因此掌握电场下水分子的迁移特性对电气设备的在线监测与危险评估有着重要意义。研究表明，在绝缘油中添加纳米粒子可以提升绝缘油的绝缘性能[13-19]，而且纳米粒子的添加可以抑制水分在绝缘油中的扩散[20]，减弱水分对绝缘纸的影响。
分子模拟技术作为一种新的研究方法，已经广泛应用于变压器油纸绝缘领域。YANG L J等[21]用分子模拟技术研究了小分子气体在矿物油和纤维素中的扩散行为。YE W Y等[22]用分子模拟技术研究了气体分子在植物油和矿物油中扩散行为的差异。LI Y Q等[23]应用分子模拟技术研究了纳米粒子和纤维素分子之间的相互作用。廖瑞金等[24]应用分子模拟技术研究了矿物油和纤维素之间的相互作用能。近年来，随着计算机科学理论和计算算法的快速发展，变压器油纸绝缘领域的分子动力学仿真技术研究也日趋成熟。
目前关于油纸绝缘中水分扩散行为的研究大多基于宏观实验，无法揭示其微观扩散行为，更无法阐述电场对水分扩散行为的影响。部分学者利用分子模拟技术研究了电场作用下水分子的扩散行为，但只是针对纯油纸系统，未考虑电场对纳米绝缘油中水分子扩散行为的影响。并且，温度和电场的协同作用会综合影响绝缘油的电气性能，更具有研究价值。因此本研究通过分子动力学方法研究在电场和温度的协同作用下纳米油中水分子的扩散行为，为纳米改性绝缘油的理论分析提供支撑。
1 模型的构建及模拟细节
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1.1 模型的构建
本研究构建了油、水和纳米SiO2粒子的共混模型，使用的仿真软件为Material Simulation分子模拟软件，油中所加的纳米粒子的质量比和半径以及水分子含量与文献[20]基本相同，而且采用相同的模拟方法。此外，本研究构建的模型以环烷基矿物绝缘油为基础 [25]，各种烷烃分子所占质量分数如表1所示，矿物油模型如图1所示；纳米SiO2粒子为团簇模型，模型中未饱和的键用H原子补足，质量分数为1%，纳米粒子半径为5 Å，如图2所示；水分子质量分数为1%，模型尺寸为64 Å×64 Å×64Å。油、水和纳米SiO2粒子的共混模型如图3所示。
1.2 模拟细节
首先用Geometry Optimizaiton对构建的共混模型进行10 000步的结构优化；当结构达到平衡后，在300～900 K下，以50 K为间隔，进行5个循环退火处理；退火后，再用Geometry Optimizaiton进行10 000步结构优化。然后，在NPT系综（即等温等压系综，系统的粒子数N、压强P和温度T保持恒定）下进行动力学计算，模拟时间为200 ps；再在电场作用下进行300 ps的NVT系综（即正则系综，系统的粒子数N、体积V和温度T保持恒定）动力学计算。电场强度设置为1010 V/m，模拟施加的电场强度远大于宏观实际值，这是因为相关研究表明在此电场强度下，电场对水分扩散行为的影响最明显[26]，并且克服了真空条件下分子的热运动，可以缩短模拟时间[27]。对动力学计算后的模型进行结构稳定判定，确定结构稳定后，进行相关计算。
2 结果与讨论
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2.1 均方位移
水分子的运动状态可以用均方位移（MSD）来表示，它描述了粒子在t时刻距初始点的平均距离。MSD由式（1）计算得到。
MSD=ri⃗t-ri⃗(0)2
式（1）中；ri⃗t和ri⃗(0) 分别表示粒子在t时刻和初始时刻的位置向量；〈〉表示对计算结果求平均值。
首先，在343 K下对构建的共混模型施加X、Y、Z 3个方向的电场，并对X、Y、Z 3个方向的均方位移进行分析，结果如图4所示。通过图4可以看出，当分别在X、Y、Z方向施加电场时，水分子的运动规律是相似的，因此，下文将以Y方向为代表。在外加电场作用下，水分子的均方位移小于文献[20]中无电场作用时水分子的均方位移。这是因为当场强达到1010 V/m时，水分子可以在极短的时间内被极化，使水分子从原本的无序排列变为有序排列。由于外加电场对水分子的束缚作用很强，因此水分子原本的布朗运动减弱。由此可见，电场作用使得
水分子在绝缘油中的扩散能力减弱。
为了探究温度和电场协同作用下温度对共混模型中水分子扩散行为的影响，对Y方向上施加电场，模拟温度在303～383 K时水分子的均方位移，结果如图5所示。从图5可以看出，在303 K下，水分子呈各向异性扩散，Y轴方向水分子的MSD明显大于X轴和Z轴方向水分子的MSD，这是因为强电场对水分子有较强的库仑推动作用力造成的。而随着温度的升高，不仅水分子总的均方位移在增加，而且X轴和Z轴与Y轴之间的差距越来越小。尤其当温度达到383 K时，在电场作用下，X、Y、Z轴之间已经没有明显差距。但是，其均方位移的数值还是远小于无电场作用时水分子在纳米油中的均
方位移，这说明相较于温度，电场对水分子扩散行为的影响更大。
2.2 自由体积
介质的自由体积是影响小粒子扩散的重要因素。根据Fox和Flory的自由体积理论[28]，自由体积计算公式如式（2）所示。
FFV=VFVF+V0
式（2）中：V0为分子占据的体积；VF为未被分子占据的自由体积。
图6为温度在343 K时模型的自由体积，其中，蓝色部分表示自由体积，灰色部分表示占有体积。通过对比可知，施加电场前后，混合模型自由体积的大小与位置都发生了明显的变化。在无电场的情况下，模型中的自由体积是连续的，并且自由体积的截面积较大。而加入电场后，模型中蓝色部分明显减少，并且多数为小的不连续的区域。
表2给出了电场作用时，不同温度下模型的自由体积分数。与文献[20]未加电场时的情况（表3）相比，电场作用下模型的自由体积分数明显减小。即使随着温度的提高，模型中自由体积分数有所增加，但还是远小于无电场作用下的自由体积分数，这表明电场对自由体积的影响要比温度对自由体积的影响更大，电场起着主要作用。究其原因，当对模型施加电场时，分子会受到强电场的作用，在某个区域沿着电场方向有序排列，水分子的运动被极大地束缚，自由体积减少。
2.3 相互作用能
水分子与油分子之间的相互作用能是影响水分子扩散行为的重要因素。相互作用能可由式（3）计算。
Eint=Etotal-(Eoil+Ewater)
式（3）中：Eint是油和水的相互作用能；Etotal是整个模型的总势能；Eoil是矿物油的势能；Ewater是水的势能。相互作用能为正值，说明物质间相互排斥；相互作用能为负值，则说明物质间相互吸引，且负值的绝对值越大，物质间结合作用越强。
模型中水分子和油分子间的能量变化是探究电场对绝缘油影响的重要因素，因此本研究对模型中水和油之间的相互作用能进行计算，并对其能量组成结构进行分析，其中两者之间的相互作用主要为范德华力和静电作用力。
表4给出了不同温度下，在施加电场时水分子与油分子间的相互作用能，表5给出了不施加电场时水分子与油分子间的相互作用能，其中Evdw代表范德华相互作用能，Eelec代表静电相互作用能。因为矿物油属于非极性物质，而水分子属于极性物质，所以两者之间的作用力主要为范德华力。对比表4和表5可以看出，在未施加电场的情况下，两者之间的相互作用能小于施加电场后的情况。这主要是因为电场引起了两者之间静电作用力的变化。施加电场后，水分子和油分子间的静电作用力是未施加电场时的2～3倍，由此说明，电场对两者间的静电作用力影响较大。
2.4 径向分布函数
分子间的作用力包括范德华作用力和氢键。图7给出了303 K和383 K下，有无电场时O原子和H原子分子间的径向分布函数（radial distribution function， RDF）。由图7可知，在1.7 Å处出现了一个明显的峰值，这是分子间氢键的作用范围，在电场作用下的峰值明显低于无电场作用时的峰值，这说明电场减弱了分子间的氢键作用。这可能是因为电场作用下水分子会沿着电场方向有序排列，从而挣脱了原有的氢键束缚。由图7还可知，随着温度的升高，RDF的峰值逐渐降低。但和无电场时RDF的峰值变化对比可知，电场作用下RDF峰值随温度的变化更小，这说明施加电场后，温度对模型中O原子和H原子之间的氢键影响减弱。
3 结论
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利用分子模拟技术研究了水分子在含有SiO2纳米粒子绝缘油中的扩散行为，通过对比有无电场时水分子在油中的扩散行为，得到如下结论：
（1）电场会束缚水分子在油中的扩散。在电场作用下，水分子沿着电场方向有序排列，减弱了水分子的布朗运动。而且在电场作用下模型中的自由体积分数、均方位移减小，导致水分子的扩散能力减弱。
（2）电场会增加水分子和油分子之间的相互作用能。外加电场时两者间的静电作用力是无电场情况下的2～3倍，范德华力无明显差别。通过径向分布函数可知，电场会减弱模型中分子间的氢键作用力。电场作用下水分子和油分子间静电作用力的增加是相互作用能增加的主要原因。
（3）电场是影响水分子在绝缘油中扩散行为的主要因素，温度对其的影响小于电场。电场作用减小了水分子的均方位移、自由体积等，增大了水分子与油介质间的静电作用力。温度升高使得径向分布函数峰值减小，但和无电场时对比，电场作用下峰值随温度的变化更小，这说明施加电场后温度对模型中O原子和H原子之间氢键的影响减弱。
基金
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  • 国家自然科学基金资助项目(51977179)
  • 中央高校基本科研业务费专项资金(XDJK2020D018)
  • 国家电网公司总部科技项目(SGKJHHJYY2018001)
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2021年第54卷第3期
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doi: 10.16790/j.cnki.1009-9239.im.2021.03.006
  • 接收时间：2020-04-26
  • 首发时间：2026-01-26
  • 出版时间：2021-02-20
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  • 收稿日期：2020-04-26
  • 修回日期：2020-06-09
基金
国家自然科学基金资助项目(51977179)
中央高校基本科研业务费专项资金(XDJK2020D018)
国家电网公司总部科技项目(SGKJHHJYY2018001)
作者信息
    1西南大学 工程技术学院，重庆 400715
    2国网重庆市电力公司电力科学研究院，重庆 401123
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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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