高导热钛酸锶/环氧树脂纳米复合材料的绝缘特性
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摘要
为研究复合材料的形貌、导热特性及电气性能,通过熔融共混法制备了填充体积分数(质量分数)分别为1.72%(7%),3.95%(15%),7.2%(25%),13.44%(40%)的钛酸锶/环氧树脂纳米复合材料。微观形貌分析表明纳米颗粒分散均匀,没有孔洞和裂痕。纳米复合材料的导热系数随着填充量的增加而增加,40%质量比复合材料的导热系数达到了0.52 W/(m·K),与纯环氧树脂相比提升了160%。复合材料的介电常数随着填充质量比的增加而增大,随着频率的增加而减小。复合材料击穿场强的Weibull分布图显示复合材料的本征击穿场强比纯环氧树脂高,增幅在25%以内。脉冲电压下沿面放电试验发现纳米复合材料沿面放电前的最高温度值低于纯环氧树脂。沿面放电电压随纳米颗粒填充量增加而显著升高,填充质量分数为40%时,沿面放电电压与纯环氧树脂相比升高了47.4%,并且具有更快的散热速率,表明填充SrTiO_3纳米颗粒可以改善环氧树脂的沿面放电特性。综上所述,填充SrTiO_3纳米颗粒的环氧树脂具有优良的导热性能和绝缘特性,为开发新型高导热绝缘材料提供了参考。
To investigated the morphology of the nanocomposites, thermal conduction characteristic and electrical properties of the composites, SrTiO_3/epoxy nanocomposites have been prepared via facile solution-processing technique by incorporating SrTiO_3 nanoparticles into the epoxy resin matrix with different loading amounts such as 1.72 vol%(7 wt%),3.95 vol%(15 wt%),7.2 vol%(25 wt%),and 13.44 vol%(40 wt%), respectively. The uniformity of dispersion in the absence of pinholes or cracks was verified in the cross-section SEM images of nanocomposites. It was found that thermal conductivity increased with SrTiO_3 weight fraction, thermal conductivity of the SrTiO_3/epoxy composite with 40% weight fraction rose up to 0.52 W/(m·K). The dielectric constant increased with the weight fraction and decreased with frequency.The Weibull distribution showed that breakdown strength of nanocomposites increased by about 25% after SrTiO_3 incorporation. Moreover, the highest temperature on the surface of samples of nanocomposites was lower than that of pure epoxy when the surface breakdown happened under impulse voltage imposition. The creeping discharge inception voltage of SrTiO_3/epoxy nanocompositeswith 40% weight fraction, compared with pure epoxy, increases by 47.4%, showing faster heat dissipation ability. Thus, adding SrTiO_3 nanoparticles can improve the creeping discharge properties of epoxy resin dielectric materials. To sum up, adding SrTiO_3/epoxy nanocomposites is beneficial to improving the thermal and dielectric properties, offering a basic reference for new insulation material development.
To investigated the morphology of the nanocomposites, thermal conduction characteristic and electrical properties of the composites, SrTiO_3/epoxy nanocomposites have been prepared via facile solution-processing technique by incorporating SrTiO_3 nanoparticles into the epoxy resin matrix with different loading amounts such as 1.72 vol%(7 wt%),3.95 vol%(15 wt%),7.2 vol%(25 wt%),and 13.44 vol%(40 wt%), respectively. The uniformity of dispersion in the absence of pinholes or cracks was verified in the cross-section SEM images of nanocomposites. It was found that thermal conductivity increased with SrTiO_3 weight fraction, thermal conductivity of the SrTiO_3/epoxy composite with 40% weight fraction rose up to 0.52 W/(m·K). The dielectric constant increased with the weight fraction and decreased with frequency.The Weibull distribution showed that breakdown strength of nanocomposites increased by about 25% after SrTiO_3 incorporation. Moreover, the highest temperature on the surface of samples of nanocomposites was lower than that of pure epoxy when the surface breakdown happened under impulse voltage imposition. The creeping discharge inception voltage of SrTiO_3/epoxy nanocompositeswith 40% weight fraction, compared with pure epoxy, increases by 47.4%, showing faster heat dissipation ability. Thus, adding SrTiO_3 nanoparticles can improve the creeping discharge properties of epoxy resin dielectric materials. To sum up, adding SrTiO_3/epoxy nanocomposites is beneficial to improving the thermal and dielectric properties, offering a basic reference for new insulation material development.
引文
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[2]李庆民,刘伟杰,韩帅,等.环氧树脂绝缘高频电热联合老化中局部放电特性分析[J].高电压技术,2015,41(2):389-395.LI Qingmin,LIU Weijie,HAN Shuai,et al.Analysis on partial discharge characteristics of epoxy resin insulation during high-frequency electrical-thermal aging[J].High Voltage Engineering,2015,41(2):389-395.
[3]ZHANG X,SHEN L,WU H,et al.Enhanced thermally conductivity and mechanical properties of polyethylene(PE)/boron nitride(BN)composites through multistage stretching extrusion[J].Composites Science&Technology,2013,89(4):24-28.
[4]LI M Q,ZHANG J J,NIU H J,et al.Effect of particle size of Al2O3 on the thermal properties of natural rubber[J].China Elastomerics,2012,3:006.
[5]江平开,陈金,黄兴溢.高导热绝缘聚合物纳米复合材料的研究现状[J].高电压技术,2017,43(9):2791-2799.JIANG Pingkai,CHEN Jin,HUANG Xingyi.Research status of thermally conductive but electrically insulating polymer nanocomposites[J].High Voltage Engineering,2017,43(9):2791-2799.
[6]LI X Y,ZHA J W,WANG S J,et al.Effect of high-thermal conductivity epoxy resin on heat dissipation performance of saturated reactor[J].IEEE Transactions on Dielectrics and Electrical Insulation,2017,24(6):3898-3905.
[7]邵千秋,孙魄韬,司马文霞,等.铜微粒对环氧树脂直流沿面闪络特性的影响[J].高电压技术,2018,44(5):1651-1659.SHAO Qianqiu,SUN Potao,SIMA Wenxia,et al.Effect of a copper particle on DC surface flashover characteristics of epoxy resin[J].High Voltage Engineering,2018,44(5):1651-1659.
[8]律方成,阴凯,付可欣,等.氟化剥离填料对氮化硼/环氧复合材料沿面闪络电压的影响[J].高电压技术,2017,43(9):2800-2807.LüFangcheng,YIN Kai,FU Kexin,et al.Effect of fluorination and exfoliation filler on the surface flashover voltage of boron nitride/epoxy resin composites[J].High Voltage Engineering,2017,43(9):2800-2807.
[9]QIANG D,WANG Y,CHEN G,et al.Dielectric properties of epoxy silica and boron nitride nanocomposites and moisture/temperature influence[J].IET Nanodielectrics,2018,1(1):48-59.
[10]QUE L,AN Z,MA Y,et al.High resistance of surface fluorinated epoxy insulators to surface discharge in SF6 gas[J].IEEE Transactions on Dielectrics and Electrical Insulation,2018,25(1):245-252.
[11]MOHAMAD A,CHEN G,CHEN Q.Investigation of plasma-enhanced-fluorination treatment on epoxy resins for high-voltage DC applications[J].IEEE Transactions on Dielectrics and Electrical Insulation,2017,24(6):3786-3793.
[12]ZHOU W,WANG C,AI T,et al.A novel fiber-reinforced polyethylene composite with added silicon nitride particles for enhanced thermal conductivity[J].Composites Part A,2009,40(6):830-836.
[13]GOJNY F H,WICHMANN M H G,FIEDLER B,et al.Evaluation and identification of electrical and thermal conduction mechanisms in carbon nanotube/epoxy composites[J].Polymer,2006,47(6):2036-2045.
[14]PARK J J,LEE J Y.Effect of epoxy-modified silicone-treated micro-/nano-silicas on the electrical breakdown strength of epoxy/silica composites[J].IEEE Transactions on Dielectrics and Electrical Insulation,2017,24(6):3794-3800.
[15]张明艳,隋珊,陈金玉,等.功能化碳纳米管/环氧树脂复合材料性能研究[J].电工技术学报,2014,29(4):97-102.ZHANG Mingyan,SUI Shan,CHEN Jinyu,et al.Study of properties of functional multi-walled carbon nanotubes/epoxy nanocomposites[J].Transactions of China Electrotechnical Society,2014,29(4):97-102.
[16]王旗,李喆,尹毅,等.微/纳米氧化铝/环氧树脂复合材料抑制电树枝生长能力的研究[J].电工技术学报,2015,30(6):255-260.WANG Qi,LI Zhe,YIN Yi,et al.The effect of micro and nano alumina on the ability of impedance on the electrical tree of epoxy resin[J].Transactions of China Electrotechnical Society,2015,30(6):255-260.
[17]KIM P,JONES S C,HOTCHKISS P J,et al.Phosphonic acid-modified barium titanate polymer nanocomposites with high permittivity and dielectric strength[J].Advanced Materials,2007,19(7):1001-1005.
[18]CHON J,YE S,CHA K J,et al.High-K dielectric sol-gel hybrid materials containing barium titanate nanoparticles[J].Chemistry of Materials,2010,22(19):5445-5452.
[19]XIE L,HUANG X,YANG K,et al.“Grafting to”route to PVDF-HFP-GMA/BaTiO3 nanocomposites with high dielectric constant and high thermal conductivity for energy storage and thermal management applications[J].Journal of Materials Chemistry A,2014,2(15):5244-5251.
[20]HUANG X Y,JIANG P K,TANAKA T.A review of dielectric polymer composites with high thermal conductivity[J].IEEE Electrical Insulation Magazine,2011,27(4):8-16.
[21]陈万平.钛酸锶和钛酸锶钡一维纳米材料的制备研究[D].湘潭:湘潭大学,2007.CHEN Wanping.Study on synthesis of one-dimensional nanomaterials of strontium titanate and barium strontium titanate[D].Xiangtan,China:Xiangtan University,2007.
[22]UVAROV N F.Estimation of composites conductivity using a general mixing rule[J].Solid State Ionics,2000(136/137):1267-1272.
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