电场下聚酰亚胺破坏的反应分子动力学模拟
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摘要
为深入研究聚酰亚胺(polyimide,PI)固体绝缘材料在电场作用下的破坏机理,采用ReaxFF(reactive force field)反应分子动力学方法,计算模拟Kapton型聚酰亚胺模型在电场作用下的破坏过程,从原子层面分析了其化学键的断裂/生成过程、特征产物的生成机理,并从原子内电荷结构的角度揭示了电场作用对化学键断裂的影响。对聚酰亚胺模拟体系外加强度分别为4、4.5、5、5.5、6×10~(-3)V/nm电场,结果表明:电场强度影响分子裂解的速度和反应的平衡状态,在电场的作用下部分化学键最终断裂,游离出大量元素单体;酰亚胺环中的C-N键是聚酰亚胺分子裂解的初始反应,电场作用下苯环断裂与裂解主要特征产物C2H2的生成有关;构成酰亚胺环中的C-N极性键的二原子在电场作用下电荷结构发生变化,产生强转矩,导致极性键断裂。电场环境下绝缘材料聚酰亚胺分子链的裂解是电气设备固体绝缘失效的主要原因。
caused disintegration of polyimide solid insulation by a Kapton-type molecular model,under electric field.From the atomic scale,the cleavage and construct of chemical bonds are analyzed with the formation mechanism of characteristic products.While,the influence of electric field effecting on broken of chemical bonds is investigated by the perspective of atomic electronic structure.The external electric field intensity is 4,4.5,5,5.5,or 6×10-3 V/nm for different simulations respectively.The result indicates that electric field intensities effects on molecular cracking reaction speed and balance state and the effect cause large number of single element free from bond order;the cleavage of polar C-N bonds in imide ring,because of the torque of C-N is strengthened by atomic electronic structure redistribution,initiate the disintegration of polyimide.The fracture of benzene ring under electric field shows a relationship of generation of C2 H2.As an insulation materials,disintegration of polyimide leads to the solid insulation failure of electrical installations.
caused disintegration of polyimide solid insulation by a Kapton-type molecular model,under electric field.From the atomic scale,the cleavage and construct of chemical bonds are analyzed with the formation mechanism of characteristic products.While,the influence of electric field effecting on broken of chemical bonds is investigated by the perspective of atomic electronic structure.The external electric field intensity is 4,4.5,5,5.5,or 6×10-3 V/nm for different simulations respectively.The result indicates that electric field intensities effects on molecular cracking reaction speed and balance state and the effect cause large number of single element free from bond order;the cleavage of polar C-N bonds in imide ring,because of the torque of C-N is strengthened by atomic electronic structure redistribution,initiate the disintegration of polyimide.The fracture of benzene ring under electric field shows a relationship of generation of C2 H2.As an insulation materials,disintegration of polyimide leads to the solid insulation failure of electrical installations.
引文
[1]张雯,张露,李家利,等.国外聚酰亚胺薄膜概况及其应用进展[J].绝缘材料,2001,34(2):21-23.ZHANG Wen,ZHANG Lu,LI Jiali,et al.Development of production and application of polyimide films broad[J].Insulating Materials,2001,34(2):21-23.
[2]章程,邵涛,于洋,等.纳秒脉冲介质阻挡放电特性及其聚合物材料表面改性[J].电工技术学报,2010,25(5):31-37.ZHANG Cheng,SHAO Tao,YU Yang,et al.Hydrophilic improvement of polymers treated by homogeneous nanosecond pulse dielectric barrier discharge in atmospheric air[J].Transactions of China Electrotechnical Society,2010,25(5):31-37.
[3]查俊伟,党智敏.聚酰亚胺/纳米ZnO耐电晕杂化膜的绝缘特性[J].中国电机工程学报,2009,24(34):122-127.ZHA Junwei,DANG Zhimin.Insulation properties of polyimide/Nano-ZnO hybrid films with good corona resistance[J].Proceedings of the CSEE,2009,24(34):122-127.
[4]SHIMOKAWA T,HAMAGUCHI Y,KAKUTA Y,et al.Effect of isothermal aging on ultimate strength of high-temperature composite materials for SST structures[J].Journal of composite materials,1999,33(12):1104-1118.
[5]汪佛池,律方成,徐志钮,等.变频电机用聚酰亚胺薄膜电老化特性研究[J].高电压技术,2007,33(4):30-32.WANG Fochi,LYU Fangcheng,XU Zhiniu,et al.Study on electrical aging characteristic of polyimide film used in frequency control motor[J].High Voltage Engineering,2007,33(4):30-32.
[6]周力任,吴广宁,高波,等.聚酰亚胺薄膜中电荷输运机理和空间电荷特性[J].电工技术学报,2009,24(12):6-11.ZHOU Liren,WU Guangning,GAO Bo,et a1.Charge transport mechanism and space charge characteristic in polyimide films[J].Transactions of China Electrotechnical Society,2009,24(12):6-11.
[7]曹开江.高频脉冲电压下牵引电机绝缘电破坏及老化机理的研究[D].成都:西南交通大学,2013.CAO Kaijiang.Electrical damage and electrical aging mechanism of traction motor insulation under high frequency pulse waveform[D].Chengdu:Southwest Jiaotong University,2013.
[8]刘洋,吴广宁,高国强,等.方波脉冲下聚酰亚胺绝缘破坏机理研究进展[J].高压电器,2016,52(7):10-18.LIU Y,WU G,GAO G,et al.Progress of research into the polyimide insulation failure mechanism under square impulse stress[J].High Voltage Apparatus,2016,52(7):10-18.
[9]张晓虹,张亮,乐波,等.基于局部放电的矩特征分析大电机主绝缘的老化[J].中国电机工程学报,2002,22(5):94-98.ZHANG Xiaohong,ZHANG Le,YUE Bo,et al.Analysis on aging condition of stator winding insulation of generator based on the moment characteristics of partial discharge[J].Proceedings of the CSEE,2002,22(5):94-98.
[10]张秀阁,胡起宙,田玉珍,等.高分子聚合物电缆绝缘电树枝老化机理浅析[J].沈阳电力高等专科学校学报,1999,1(4):10-14.ZHANG Xiuge,HU Qizhou,TIAN Yuzhen,et al.An analysis of high molecule insulation materials electrical tree aging mechanism[J].Journal of Shenyang Electric Power Institute,1999,1(4):10-14.
[11]VAN DUIN A C,DASGUPTA S,LORANT F,et al.ReaxFF:A reactive force field for hydrocarbons[J].the Journal of Physical Chemistry A,2001,105(41):9396-9409.
[12]VAN DUIN A C,ZEIRI Y,DUBNIKOVA F,et al.Atomistic-scale simulations of the initial chemical events in the thermal initiation of triacetonetriperoxide[J].Journal of the American Chemical Society,2005,127(31):11053-11062.
[13]NOMURA K,KALIA R K,NAKANO A,et al.Dynamic transition in the structure of an energetic crystal during chemical reactions at shock front prior to detonation[J].Physical Review Letters,2007,99(14):148-303.
[14]TAKEUCHI A,INOUE A.Calculations of mixing enthalpy and mismatch entropy for ternary amorphous alloys[J].Materials Transactions on JIM,2000,41(11):1372-1378.
[15]CHENOWETH K,CHEUNG S,VAN DUIN A C,et al.Simulations on the thermal decomposition of a poly(dimethylsiloxane)polymer using the ReaxFF reactive force field[J].Journal of the American Chemical Society,2005,127(19):7192-7202.
[16]RAHNAMOUN A,VAN DUIN A C.Reactive molecular dynamics simulation on the disintegration of kapton,POSSpolyimide,amorphous silica,and teflon during atomic oxygen impact using the reaxff reactive force-field method[J].the Journal of Physical Chemistry A,2014,118(15):2780-2787.
[17]LU X,WANG X,LI Q,et al.A ReaxFF-based molecular dynamics study of the pyrolysis mechanism of polyimide[J].Polymer Degradation and Stability,2015(114):72-80.
[18]ISLAM M M,BRYANTSEV V S,VAN DUIN A C.ReaxFFreactive force field simulations on the influence of teflon on electrolyte decomposition during Li/SWCNT anode discharge in lithium-sulfur batteries[J].Journal of the Electrochemical Society,2014,161(8):3009-3014.
[19]GUBBELS-ELZAS A,THIJSSE B J.Ionic motion during field-assisted oxidation of aluminium studied by molecular dynamics simulations[J].Computational Materials Science,2014(90):196-202.
[20]LI H,REN D,CHENG X.The theoretical investigation of theβ-crystobalite structure under the effect of electric field[J].Computational Materials Science,2015(96):306-311.
[21]刘连池.ReaxFF反应力场的开发及其在材料科学中的若干应用[D].上海:上海交通大学,2012.LIU Lianchi,Development of Reax FF reactive force field and several applications in materials science[D].Shanghai:Shanghai Jiao Tong University,2012.
[22]RUSSO M F,VAN DUIN A C.Atomistic-scale simulations of chemical reactions:Bridging from quantum chemistry to engineering[J].Nuclear Instruments and Methods in Physics Research Section B:Beam Interactions with Materials and Atoms,2011,269(14):1549-1554.
[23]SHABMA B L,PILLAI P K C.Photoconduction in kapton polyimide film at high electric fields[J].Physica Status Solidi(A),1982,71(2):583-588.
[24]BELANA J,CANADAS J C,DIEGO J A,et al.Physical ageing studies in polyetherimide ULTEM 1000[J].Polymer international,1998,46(1):29-32.
[25]INAGAKI M,SAKAMOTO K,HISHIYAMA Y.Carbonization and graphitization of polyimide upilex[J].Journal of Materials Research,1991,6(5):1108-1113.
[26]HATORI H,YAMADA Y,SHIRAISHI M,et al.The mechanism of polyimide pyrolysis in the early stage[J].Carbon,1996,34(2):201-208.
[2]章程,邵涛,于洋,等.纳秒脉冲介质阻挡放电特性及其聚合物材料表面改性[J].电工技术学报,2010,25(5):31-37.ZHANG Cheng,SHAO Tao,YU Yang,et al.Hydrophilic improvement of polymers treated by homogeneous nanosecond pulse dielectric barrier discharge in atmospheric air[J].Transactions of China Electrotechnical Society,2010,25(5):31-37.
[3]查俊伟,党智敏.聚酰亚胺/纳米ZnO耐电晕杂化膜的绝缘特性[J].中国电机工程学报,2009,24(34):122-127.ZHA Junwei,DANG Zhimin.Insulation properties of polyimide/Nano-ZnO hybrid films with good corona resistance[J].Proceedings of the CSEE,2009,24(34):122-127.
[4]SHIMOKAWA T,HAMAGUCHI Y,KAKUTA Y,et al.Effect of isothermal aging on ultimate strength of high-temperature composite materials for SST structures[J].Journal of composite materials,1999,33(12):1104-1118.
[5]汪佛池,律方成,徐志钮,等.变频电机用聚酰亚胺薄膜电老化特性研究[J].高电压技术,2007,33(4):30-32.WANG Fochi,LYU Fangcheng,XU Zhiniu,et al.Study on electrical aging characteristic of polyimide film used in frequency control motor[J].High Voltage Engineering,2007,33(4):30-32.
[6]周力任,吴广宁,高波,等.聚酰亚胺薄膜中电荷输运机理和空间电荷特性[J].电工技术学报,2009,24(12):6-11.ZHOU Liren,WU Guangning,GAO Bo,et a1.Charge transport mechanism and space charge characteristic in polyimide films[J].Transactions of China Electrotechnical Society,2009,24(12):6-11.
[7]曹开江.高频脉冲电压下牵引电机绝缘电破坏及老化机理的研究[D].成都:西南交通大学,2013.CAO Kaijiang.Electrical damage and electrical aging mechanism of traction motor insulation under high frequency pulse waveform[D].Chengdu:Southwest Jiaotong University,2013.
[8]刘洋,吴广宁,高国强,等.方波脉冲下聚酰亚胺绝缘破坏机理研究进展[J].高压电器,2016,52(7):10-18.LIU Y,WU G,GAO G,et al.Progress of research into the polyimide insulation failure mechanism under square impulse stress[J].High Voltage Apparatus,2016,52(7):10-18.
[9]张晓虹,张亮,乐波,等.基于局部放电的矩特征分析大电机主绝缘的老化[J].中国电机工程学报,2002,22(5):94-98.ZHANG Xiaohong,ZHANG Le,YUE Bo,et al.Analysis on aging condition of stator winding insulation of generator based on the moment characteristics of partial discharge[J].Proceedings of the CSEE,2002,22(5):94-98.
[10]张秀阁,胡起宙,田玉珍,等.高分子聚合物电缆绝缘电树枝老化机理浅析[J].沈阳电力高等专科学校学报,1999,1(4):10-14.ZHANG Xiuge,HU Qizhou,TIAN Yuzhen,et al.An analysis of high molecule insulation materials electrical tree aging mechanism[J].Journal of Shenyang Electric Power Institute,1999,1(4):10-14.
[11]VAN DUIN A C,DASGUPTA S,LORANT F,et al.ReaxFF:A reactive force field for hydrocarbons[J].the Journal of Physical Chemistry A,2001,105(41):9396-9409.
[12]VAN DUIN A C,ZEIRI Y,DUBNIKOVA F,et al.Atomistic-scale simulations of the initial chemical events in the thermal initiation of triacetonetriperoxide[J].Journal of the American Chemical Society,2005,127(31):11053-11062.
[13]NOMURA K,KALIA R K,NAKANO A,et al.Dynamic transition in the structure of an energetic crystal during chemical reactions at shock front prior to detonation[J].Physical Review Letters,2007,99(14):148-303.
[14]TAKEUCHI A,INOUE A.Calculations of mixing enthalpy and mismatch entropy for ternary amorphous alloys[J].Materials Transactions on JIM,2000,41(11):1372-1378.
[15]CHENOWETH K,CHEUNG S,VAN DUIN A C,et al.Simulations on the thermal decomposition of a poly(dimethylsiloxane)polymer using the ReaxFF reactive force field[J].Journal of the American Chemical Society,2005,127(19):7192-7202.
[16]RAHNAMOUN A,VAN DUIN A C.Reactive molecular dynamics simulation on the disintegration of kapton,POSSpolyimide,amorphous silica,and teflon during atomic oxygen impact using the reaxff reactive force-field method[J].the Journal of Physical Chemistry A,2014,118(15):2780-2787.
[17]LU X,WANG X,LI Q,et al.A ReaxFF-based molecular dynamics study of the pyrolysis mechanism of polyimide[J].Polymer Degradation and Stability,2015(114):72-80.
[18]ISLAM M M,BRYANTSEV V S,VAN DUIN A C.ReaxFFreactive force field simulations on the influence of teflon on electrolyte decomposition during Li/SWCNT anode discharge in lithium-sulfur batteries[J].Journal of the Electrochemical Society,2014,161(8):3009-3014.
[19]GUBBELS-ELZAS A,THIJSSE B J.Ionic motion during field-assisted oxidation of aluminium studied by molecular dynamics simulations[J].Computational Materials Science,2014(90):196-202.
[20]LI H,REN D,CHENG X.The theoretical investigation of theβ-crystobalite structure under the effect of electric field[J].Computational Materials Science,2015(96):306-311.
[21]刘连池.ReaxFF反应力场的开发及其在材料科学中的若干应用[D].上海:上海交通大学,2012.LIU Lianchi,Development of Reax FF reactive force field and several applications in materials science[D].Shanghai:Shanghai Jiao Tong University,2012.
[22]RUSSO M F,VAN DUIN A C.Atomistic-scale simulations of chemical reactions:Bridging from quantum chemistry to engineering[J].Nuclear Instruments and Methods in Physics Research Section B:Beam Interactions with Materials and Atoms,2011,269(14):1549-1554.
[23]SHABMA B L,PILLAI P K C.Photoconduction in kapton polyimide film at high electric fields[J].Physica Status Solidi(A),1982,71(2):583-588.
[24]BELANA J,CANADAS J C,DIEGO J A,et al.Physical ageing studies in polyetherimide ULTEM 1000[J].Polymer international,1998,46(1):29-32.
[25]INAGAKI M,SAKAMOTO K,HISHIYAMA Y.Carbonization and graphitization of polyimide upilex[J].Journal of Materials Research,1991,6(5):1108-1113.
[26]HATORI H,YAMADA Y,SHIRAISHI M,et al.The mechanism of polyimide pyrolysis in the early stage[J].Carbon,1996,34(2):201-208.
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