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Article(id=1222482749873709203, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1222482747264852071, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2021.01.005, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1587916800000, receivedDateStr=2020-04-27, revisedDate=1593446400000, revisedDateStr=2020-06-30, acceptedDate=null, acceptedDateStr=null, onlineDate=1769392200200, onlineDateStr=2026-01-26, pubDate=1611072000000, pubDateStr=2021-01-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1769392200200, onlineIssueDateStr=2026-01-26, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1769392200200, creator=13041195026, updateTime=1769392200200, updator=13041195026, issue=Issue{id=1222482747264852071, tenantId=1146029695717560320, journalId=1149653034449285133, year='2021', volume='54', issue='1', 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=1769392199579, creator=13041195026, updateTime=1769414905563, updator=13041195026, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1222577983139861118, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1222482747264852071, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1222577983144055423, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1222482747264852071, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=25, endPage=30, ext={EN=ArticleExt(id=1222482750213447840, articleId=1222482749873709203, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Influence of KH550 Grafting Density on Surface of Nano-SiO2 on Mechanical Properties and Thermal Stability of Modified Cellulose Insulating Paper, columnId=1190369066675179686, journalTitle=Insulating Materials, columnName=Material Research, runingTitle=null, highlight=null, articleAbstract=

In order to improve the mechanical properties and thermal stability of cellulose insulating paper, the nano-SiO2, surface modified by KH550, was doped into cellulose insulating paper. The nano-SiO2/cellulose composite models with different grafting density were established through molecular simulation, and their mechanical properties, mean square displacement, cohesive energy density, solubility parameter, and radial distribution function were calculated and analyzed. The results show that when the grafting density of KH550 is 12.5%, the nano-SiO2/cellulose composite system has optimum deformation resistance, large cohesive energy density and solubility parameter.

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为提升纤维素绝缘纸的力学性能与热稳定性，利用KH550对纳米SiO2进行表面改性，将其掺杂到纤维素绝缘纸中，通过分子模拟建立不同接枝密度的纳米SiO2/纤维素复合模型，并对各模型的力学性能、均方位移、内聚能密度、溶解度参数和径向分布函数进行计算和分析。结果表明：KH550接枝密度为12.5%的纳米SiO2/纤维素复合模型抗形变能力最佳，并具有较大的内聚能密度和溶解度参数，改性效果最佳。

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唐超（1981-），男（汉族），四川自贡人，教授，博士，研究方向为电气设备在线监测、故障诊断及状态评价技术。
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杨路（1996-），女（汉族），山西长治人，硕士生，研究方向为变压器绝缘纸的性能与改性。

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杨路（1996-），女（汉族），山西长治人，硕士生，研究方向为变压器绝缘纸的性能与改性。

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杨路（1996-），女（汉族），山西长治人，硕士生，研究方向为变压器绝缘纸的性能与改性。

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模型体积模量(K)剪切模量(G)泊松比(v)弹性模量(E)K/G柯西压(C12-C44)
Pure7.073 04.459 20.239 58.374 61.518 6-1.200 3
3%-SiO27.064 44.265 60.248 78.070 11.656 1-0.321 5
9%-SiO28.384 55.132 60.245 89.688 01.633 6-1.061 4
12%-SiO29.865 25.522 90.264 110.577 91.786 2-0.120 6
15%-SiO28.664 54.687 30.243 910.242 61.848 5-1.117 6
18%-SiO28.438 84.551 50.241 49.573 81.854 0-1.081 6
), ArticleFig(id=1222577745574482394, tenantId=1146029695717560320, journalId=1149653034449285133, articleId=1222482749873709203, language=CN, label=表1, caption=

各模型在343 K下的力学性能参数

, figureFileSmall=null, figureFileBig=null, tableContent=
模型体积模量(K)剪切模量(G)泊松比(v)弹性模量(E)K/G柯西压(C12-C44)
Pure7.073 04.459 20.239 58.374 61.518 6-1.200 3
3%-SiO27.064 44.265 60.248 78.070 11.656 1-0.321 5
9%-SiO28.384 55.132 60.245 89.688 01.633 6-1.061 4
12%-SiO29.865 25.522 90.264 110.577 91.786 2-0.120 6
15%-SiO28.664 54.687 30.243 910.242 61.848 5-1.117 6
18%-SiO28.438 84.551 50.241 49.573 81.854 0-1.081 6
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纳米SiO2表面KH550接枝密度对改性纤维素绝缘纸力学性能与热稳定性的影响
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杨路 1 , 庞锴 2 , 王栋 2 , 孙鹏 2 , 邱秦攀 1 , 唐超 1
绝缘材料 | 材料研究 2021,54(1): 25-30
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绝缘材料 | 材料研究 2021, 54(1): 25-30
纳米SiO2表面KH550接枝密度对改性纤维素绝缘纸力学性能与热稳定性的影响
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杨路1, 庞锴2, 王栋2, 孙鹏2, 邱秦攀1, 唐超1
作者信息
  • 1西南大学 工程技术学院，重庆 400700
  • 2国网河南省电力公司电力科学研究院，河南 郑州 450000

    • 杨路（1996-），女（汉族），山西长治人，硕士生，研究方向为变压器绝缘纸的性能与改性。

通讯作者:

唐超（1981-），男（汉族），四川自贡人，教授，博士，研究方向为电气设备在线监测、故障诊断及状态评价技术。
Influence of KH550 Grafting Density on Surface of Nano-SiO2 on Mechanical Properties and Thermal Stability of Modified Cellulose Insulating Paper
Lu YANG1, Kai PANG2, Dong WANG2, Peng SUN2, Qinpan QIU1, Chao TANG1
Affiliations
  • 1College of Engineering and Technology, Southwest University, Chongqing 400700, China
  • 2Electric Power Research Institute of State Grid Henan Electric Power Company, Zhengzhou 450000, China
出版时间: 2021-01-20 doi: 10.16790/j.cnki.1009-9239.im.2021.01.005
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摘要
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为提升纤维素绝缘纸的力学性能与热稳定性，利用KH550对纳米SiO2进行表面改性，将其掺杂到纤维素绝缘纸中，通过分子模拟建立不同接枝密度的纳米SiO2/纤维素复合模型，并对各模型的力学性能、均方位移、内聚能密度、溶解度参数和径向分布函数进行计算和分析。结果表明：KH550接枝密度为12.5%的纳米SiO2/纤维素复合模型抗形变能力最佳，并具有较大的内聚能密度和溶解度参数，改性效果最佳。

硅烷偶联剂KH550  /  纤维素绝缘纸  /  纳米SiO2  /  接枝密度

In order to improve the mechanical properties and thermal stability of cellulose insulating paper, the nano-SiO2, surface modified by KH550, was doped into cellulose insulating paper. The nano-SiO2/cellulose composite models with different grafting density were established through molecular simulation, and their mechanical properties, mean square displacement, cohesive energy density, solubility parameter, and radial distribution function were calculated and analyzed. The results show that when the grafting density of KH550 is 12.5%, the nano-SiO2/cellulose composite system has optimum deformation resistance, large cohesive energy density and solubility parameter.

silane coupling agent KH550  /  cellulose insulating paper  /  nano-SiO2  /  grafting density
杨路, 庞锴, 王栋, 孙鹏, 邱秦攀, 唐超. 纳米SiO2表面KH550接枝密度对改性纤维素绝缘纸力学性能与热稳定性的影响. 绝缘材料, 2021 , 54 (1) : 25 -30 . DOI: 10.16790/j.cnki.1009-9239.im.2021.01.005
Lu YANG, Kai PANG, Dong WANG, Peng SUN, Qinpan QIU, Chao TANG. Influence of KH550 Grafting Density on Surface of Nano-SiO2 on Mechanical Properties and Thermal Stability of Modified Cellulose Insulating Paper[J]. Insulating Materials, 2021 , 54 (1) : 25 -30 . DOI: 10.16790/j.cnki.1009-9239.im.2021.01.005
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0 引言
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绝缘纸的性能是影响电力变压器性能的重要因素，为提升绝缘纸性能，利用新兴的纳米技术对绝缘纸纤维素进行改性是变压器绝缘研究的热点。目前，纳米粒子修饰纤维素已有很多成熟的研究，如张松等[1]利用纳米Al2O3对纤维素绝缘纸进行改性，发现改性后的绝缘纸具有优异的强度与韧性；GAO Fei等[2]利用纳米Al2O3改善了纤维素绝缘纸的电性能；HAO Jian等[3]利用纳米PTFE对绝缘纸的纤维素覆膜进行改性以提高其击穿电压和改善其疏水性；LIAO Ruijin等[4]利用TiO2对油浸绝缘纸纤维素进行改性，提升了纤维素绝缘纸的拉伸强度、电气强度和介电性能；TANG Chao等[5]利用纳米SiO2粒子进行改性，提高了纤维素绝缘纸的拉伸强度和玻璃化转变温度。可见，利用纳米粒子进行改性可以有效改善纤维素绝缘纸的性能。
一些纳米粒子表面含有羟基，易与水分子发生反应而团聚，使其对材料性能的改善作用无法充分发挥，因此通常利用偶联剂对纳米粒子表面进行处理，其中硅烷偶联剂能对含羟基的纳米粒子进行有效的表面改性 [6-7]。朱子沛等[8]利用硅烷偶联剂改性纳米Al2O3，减少了纳米粒子的团聚现象，提高了材料的力学性能，优化了杂交膜的形貌。V PURCAR等[9]利用不同的硅烷偶联剂通过溶胶-凝胶法合成了以纳米氧化锌为基础的杂化纳米复合材料，该复合材料的热稳定性得到了提升，并且表面接触角增大，可用于防腐蚀和防冰涂料。LI Dongna等[10]用KH570接枝纳米SiO2，改性后的材料分散更加均匀，最大热分解温度和结晶度提高。本课题组[11-12]选用KH550与KH792对纳米SiO2进行了改性，改性后的材料性能较佳，其中KH550在硅烷偶联剂中由于价格相对低廉而受到广泛应用。
随着计算机技术的发展，分子模拟技术已经广泛应用于分子微观机理的推算和研究[13]。WEI Qinghua等[14]采用分子动力学方法研究了纳米SiO2粒子对聚乙烯醇/聚乙烯吡咯烷酮共混体系性能的影响，揭示了纳米SiO2粒子在共混体系中的相互作用机理；M MOHAMMADI等[15]采用分子动力学模拟方法研究了氧化铝纳米颗粒对聚甲基丙烯酸甲酯（is-PMMA）聚合物热扩散性能的影响；K BYUNGJO等[16]采用分子动力学模拟方法研究了不同交联度的环氧树脂（EP）掺杂不同尺寸纳米SiO2后的力学性能和热稳定性。
综上，目前纳米SiO2的掺杂[17-18]和KH550[19-21]的接枝对纤维素绝缘纸的改性效果得到了广泛的认可，但是对硅烷偶联剂修饰纳米SiO2提升纤维素绝缘纸的微观机理并没有得到很好的解释。
本研究基于分子动力学建立不同接枝密度的硅烷偶联剂接枝的纳米SiO2/纤维素模型，并对模型的力学性能、径向分布函数（RDF）、内聚能密度（CED）、溶解度参数（SP）和均方位移（MSD）进行计算和分析，研究硅烷偶联剂在纳米SiO2改性纤维素绝缘纸的过程机理。
1 模型搭建及参数设置
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在Materials Studio（MS）软件的Amorphous cell（AC）模块中分别建立纤维素聚合度（DP）为10、初始密度为0.6 g/cm3的纤维素模型，以及KH550接枝密度[22]分别为0、3.12%、9.37%、12.5%、15.6%、18.75%的纳米SiO2/纤维素复合模型[23]，分别记为Pure、3%-SiO2、9%-SiO2、12%-SiO2、15%-SiO2、18%-SiO2。在MS软件中先建立纤维素、硅烷偶联剂（KH550）以及纳米SiO2的模型，利用图1所示的水解反应在已羟基化的纳米SiO2表面接枝硅烷偶联剂，再在Amorphous cell模块中使用packing方法构建纤维素与改性纳米SiO2的复合模型。
对模型进行几何优化，利用Forcite模块进行步长为1 fs、总步数为5 000步的能量最小化计算，再进行温度为300～900 K的5个循环的退火处理，选择能量最小的结构模型再次进行5 000步的结构优化和能量最小化计算。接着对模型进行分子动力学模拟：先后进行300 ps、500 ps的NPT模拟计算（压力为1 atm）。在能量优化以及分子动力学模拟过程中，采用Compass力场[24]、Nose控温方法[25]和Ewald静电方法，Vander Waals作用采用AtomBased方法，压强控制采用Berendsen方法，模型如图2所示。
2 分析和讨论
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2.1 力学性能
纤维素体系沿着x-x、y-y、z-z、y-z、x-z和x-y平面产生剪切变形，其应力应变关系满足胡克定律，如式（1）～（2）所示。
σi=Cijεj
σ1σ2σ3σ4σ5σ6=C11C12C13C14C15C16C21C22C23C24C25C26C31C32C33C34C35C36C41C42C43C44C45C46C51C52C53C54C55C56C61C62C63C64C65C66⋅ε1ε2ε3ε4ε5ε6
式（1）～（2）中：σi为应力；Cij为计算所得的弹性刚度系数矩阵；εj为应变张量[26]。
复合材料的弹性模量E、剪切模量G、体积模量K和泊松比v分别可以用弹性常量λ和μ表示，如式（3）～（6）所示。
E=μ⋅3λ+2μλ+μ
G=μ
K=λ+23μ
ν=λ2(λ+μ)
表1给出了6个模型在343 K下的体积模量K、剪切模量G、泊松比v、弹性模量E、K/G和柯西压值（C12-C44）。体积模量K可以反映材料的宏观力学特性，是体现物体应变和平均应力关系的物理量；剪切模量G又称切变模量，是剪切应力与应变的比值；泊松比v也叫横向变形系数，是反映材料横向变形的弹性系数；弹性模量E又称杨氏模量，表征材料抗形变的能力，其值越大，材料抗形变的能力越强；K/G值是体积模量K与剪切模量G的比值，用于评价材料的韧性；柯西压是衡量材料延展性的参数，其值越大表示材料延展性越好，其值越小表示材料越脆。
从表1可以看出，经KH550改性后，接枝KH550的模型在各个力学参数上基本都有所改善，其中3%-SiO2的脆性提升最大，12%-SiO2的力学性能提升最大。这是由于在硅烷偶联剂接枝密度低于12.5%时，随着接枝密度的增加，分子间的范德华力增大，分子间的纠缠效应也增强，模型的力学性能得到提升。当接枝密度超过12.5%以后，纳米SiO2表面的硅烷偶联剂之间的空间距离变小，纤维素链难以进入到硅烷偶联剂的空隙中，微观力学互锁效应减弱，导致其力学性能下降，这与文献[27]得到的结论接近。
2.2 均方位移
为了探究KH550改性纳米SiO2对纤维素链运动能力的影响，用均方位移（MSD）来表征纤维素链热运动的位移，均方位移的值越大，物体热运动越剧烈。均方位移[28-31]的值可以通过式（7）计算。
MSD=ri(t)-ri(0)2
式（7）中：ri(t)为t时刻i分子或原子的位置；ri(0)表示0时刻i分子或原子的位置。
图3为各模型在343 K下纤维素链的均方位移。从图3可以看出，未经KH550改性的纤维素模型均方位移变化范围为0～10 Å2，3%-SiO2、9%-SiO2、12%-SiO2、15%-SiO2、18%-SiO2的均方位移变化范围分别为0～5.1 Å2、0～4.6 Å2、0～3.79 Å2、0～6.41 Å2、0～8.9 Å2。改性模型的均方位移均小于未改性模型，这是因为KH550接枝纳米SiO2后与纤维素链形成了更多的氢键，减缓了纤维素链的热运动。12%-SiO2纤维素链的均方位移变化范围最小，而15%-SiO2和18%-SiO2的均方位移相对于12%-SiO2有所上升，这是因为在高接枝密度的情况下，纤维素链较难进入到硅烷偶联剂之间的空隙，纳米SiO2对纤维素链的束缚力减弱。
2.3 内聚能密度和溶解度参数
高分子聚合物之间的作用力通常用内聚能或者内聚能密度[32-33]表示，主要反映基团间的相互作用。内聚能（CED）通常指一个分子体系中所有分子分离到无限远处所需要的平均能量，分子间作用力越大，体系的内聚能就越大，其计算如式（8）所示。
CED=EceV=Etotal-EintraV=EinterV
式（8）中：Ece表示体系的内聚能；Etotal表示体系的总能量；Eintra表示分子内的能量；Einter表示分子间的能量；V表示体系的体积。
溶解度参数（SP）可用于表征体系内分子间相互作用强度的大小，现已作为物质间相容性判断的一个重要参数，其计算如式（9）所示。
SP=CED
图4为各模型的内聚能密度和溶解度参数。由图4可以看出，模型内聚能密度为450～700 J/cm3，这代表着模型中分子链有极强的极性基团或者分子间能形成氢键。接枝KH550的模型比未接枝模型的内聚能密度均有上升，说明在纳米SiO2表面接枝KH550与纤维素链之间形成了更多的氢键，增大了纤维素链与纳米SiO2的结合能。CED和SP值均随着接枝密度的增加先增大再减小，这是因为在接枝密度较大时，KH550在纳米SiO2表面互相靠近，形成半封闭的空间结构，使纤维素分子链不易渗透到纳米SiO2表面与极性较强的基团形成氢键，导致体系的结合能降低，相容性变差。
2.4 径向分布函数
两组分之间的相互作用可以通过径向分布函数来反映，径向分布函数[34-35]表示在完全随机分布的体系中，基团A的r距离内出现基团B的概率密度（gAB(r)），可表示为式（10）。
gAB(r)=∑i≠jδ(r-rAi-rBi)(NANB-NAB)4πr2dr
式（10）中：i和j表示基团A和基团B中的第i和第j个原子；NAB表示基团A和基团B的总原子数。
通常可以从径向分布函数（RDF）曲线中峰的位置判断两种基团之间的距离，从峰值判断两种原子作用的强度。图5为不同模型在343 K下的RDF曲线及其在0～3 Å峰值的放大图。从图5可以看出，这几种模型的RDF曲线相似，在短距离内为0，在5 Å以上趋于稳定。一般在3.5 Å以下的峰值主要体现化学键和氢键的强弱，而3.5 Å以上的峰值对应范德华力和静电力的强弱。
图5中，第一和第二个峰出现在0.8～1.2 Å，这是氢和其他原子之间的化学键造成的，其中以氢键为主要因素。6个模型中12%-SiO2在第一个和第二个峰的峰值最高，分别为2.8和2.6。第三个峰出现在1.3～1.7 Å，这是C原子与其相连的原子形成的键（例如C-O、C-N键）造成的。第四个峰和第五个峰出现在1.9～2.3 Å和2.4～2.6 Å，这是体系中相隔两个键的化学键（例如C-C-C和C-C-H）和3个原子以上所构成的化学键生成的。在本研究构造的模型中，经过KH550改性的模型RDF峰值均比未改性的模型要大，这表明在改性后的体系中形成了更多的化学键与氢键，分子间具有更强的相互作用。其中12%-SiO2由于模型结构最为优异而拥有最多的氢键，所以峰值也最高。当接枝密度较大时，峰值随着接枝密度的增大反而下降，也可以印证之前接枝密度过大不利于形成更优异的体系结构进而导致材料性能下降的结论。
3 结论
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（1）相对于未接枝KH550的纳米SiO2/纤维素体系，接枝KH550后的纳米SiO2能提升纳米SiO2/纤维素体系的力学性能，减缓体系中纤维素链运动，增大分子间的相互作用，提高相容性，进而有效提升纳米SiO2/纤维素体系的热稳定性。
（2）对于不同接枝密度的KH550改性纳米SiO2/纤维素体系，KH550接枝密度为12.5%时，改性纳米SiO2/纤维素体系的力学性能、RDF、内聚能密度、溶解度参数和MSD相对最佳，其中MSD降低了约 6 Å2，内聚能密度提高了33%，溶解度参数提高了15%，且表面结构更为优异。因此对于接枝KH550的纳米SiO2/纤维素体系而言，选择12.5%的接枝密度能获得最佳的改性效果。
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资助项目(XDJK2020D018)
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2021年第54卷第1期
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doi: 10.16790/j.cnki.1009-9239.im.2021.01.005
  • 接收时间：2020-04-27
  • 首发时间：2026-01-26
  • 出版时间：2021-01-20
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  • 收稿日期：2020-04-27
  • 修回日期：2020-06-30
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资助项目(XDJK2020D018)
作者信息
    1西南大学 工程技术学院，重庆 400700
    2国网河南省电力公司电力科学研究院，河南 郑州 450000

通讯作者:

唐超（1981-），男（汉族），四川自贡人，教授，博士，研究方向为电气设备在线监测、故障诊断及状态评价技术。
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https://castjournals.cast.org.cn/joweb/jycl/CN/10.16790/j.cnki.1009-9239.im.2021.01.005
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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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