氮化硼纳米片/银纳米杂化颗粒填充的环氧树脂复合材料的制备及其性能研究
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摘要
填充型高导热聚合物复合材料是目前解决电子器件散热问题的重要材料。基于此,该文通过液相剥离和化学还原法制备了氮化硼纳米片/银纳米粒子(BNNSs/AgNPs)杂化粒子,并以此为填料制备了BNNSs/AgNPs/环氧树脂复合材料。前期研究工作证实通过BNNSs/AgNPs杂化粒子的填充,复合材料的导热性能得到了有效提高。然而,复合材料其他方面的综合性能也相当重要。因此,通过热失重、动态热机械性能以及介电性能测试对BNNSs/AgNPs/环氧树脂复合体系的电学和力学性能进行考察和分析。结果表明,杂化粒子的填充对复合材料热分解温度有所提高,复合物的介电常数随着填料含量的增加而增加,BNNSs/AgNPs/环氧树脂的介电常数相对于BNNSs/环氧树脂有进一步的提高。复合材料的储能模量和玻璃化转变温度随着填料含量的增加而升高。相对于BNNSs,BNNSs/AgNPs杂化粒子使得环氧树脂复合物的玻璃化转变温度进一步提高。BNNSs/AgNPs/环氧树脂复合材料良好的热学、力学和电学性能,能进一步满足聚合物基复合材料在现代电子器件和设备封装领域的要求。
Filled high thermally conductive polymer composites will be vital materials to resolve heat dissipation problem in electronics. Herein, boron nitride nanosheet/silver nanoparticles(BNNSs/AgNPs) hybrids were prepared through liquid exfoliation and chemical reduction method, and then were added into epoxy resin(EP) to prepare BNNSs/AgNPs/EP composites. Previous study has proved that the thermal conductivities of the composites were enhanced with the addition of the BNNSs/AgNPs hybrids. Further, the over-all properties are also important to evaluate the performance of the polymer composites. In this paper, electrical and mechanical properties of the BNNSs/AgNPs/EP composites were investigated by thermogravimetric analysis, dynamic thermomechanical analysis and dielectric strength measurement. The result shows that the decomposed temperature is increased with the addition of BNNSs/AgNPs hybrids, the dielectric constant is increased with the increase of the filler content, and the dielectric constant of BNNSs/AgNPs/EP is higher than that of BNNSs/EP. Energy storage modulus and glass transition temperature are both increased with increasing the filler content. Compared with BNNSs, impregnation of BNNSs/AgNPs hybrids to the EP makes the composite with higher glass transition temperature. The results indicate that the obtained BNNSs/AgNPs/EP composites, possessing good thermal, electrical and mechanical properties, will meet the requirement in modern electronics packaging field.
Filled high thermally conductive polymer composites will be vital materials to resolve heat dissipation problem in electronics. Herein, boron nitride nanosheet/silver nanoparticles(BNNSs/AgNPs) hybrids were prepared through liquid exfoliation and chemical reduction method, and then were added into epoxy resin(EP) to prepare BNNSs/AgNPs/EP composites. Previous study has proved that the thermal conductivities of the composites were enhanced with the addition of the BNNSs/AgNPs hybrids. Further, the over-all properties are also important to evaluate the performance of the polymer composites. In this paper, electrical and mechanical properties of the BNNSs/AgNPs/EP composites were investigated by thermogravimetric analysis, dynamic thermomechanical analysis and dielectric strength measurement. The result shows that the decomposed temperature is increased with the addition of BNNSs/AgNPs hybrids, the dielectric constant is increased with the increase of the filler content, and the dielectric constant of BNNSs/AgNPs/EP is higher than that of BNNSs/EP. Energy storage modulus and glass transition temperature are both increased with increasing the filler content. Compared with BNNSs, impregnation of BNNSs/AgNPs hybrids to the EP makes the composite with higher glass transition temperature. The results indicate that the obtained BNNSs/AgNPs/EP composites, possessing good thermal, electrical and mechanical properties, will meet the requirement in modern electronics packaging field.
引文
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[2]周文英,丁小卫.导热高分子材料[M].北京:国防工业出版社,2014.
[3]Wu XF,Wang Y,Xie LY,et al.Thermal and electrical properties of epoxy composites at high alumina loadings and various temperatures[J].Iranian Polymer Journal,2013,22(1):61-73.
[4]Tang DH,Su JQ,Yang Q,et al.Preparation of alumina-coated graphite for thermally conductive and electrically insulating epoxy composites[J].RSC Advances,2015,5(68):55170-55178.
[5]Sato K,Ijuin A,Hotta Y.Thermal conductivity enhancement of alumina/polyamide composites via interfacial modification[J].Ceramics International,2015,41(8):10314-10318.
[6]Liu MD,Jia K,Liu XB.Effective thermal phthalonitrile-terminated poly(arylene ether nitriles)composites with hybrid functionalized alumina[J].Journal of Applied Polymer Science,2015,132(10):41595-41602.
[7]Shi ZQ,Radwan M,Kirihara S,et al.Enhanced thermal conductivity of polymer composites filled with three-dimensional brushlike AlN nanowhiskers[J].Applied Physics Letters,2009,95(22):282-289.
[8]Cao JP,Zhao XD,Zhao J,et al.Improved thermal conductivity and flame retardancy in polystyrene/poly(vinylidene fluoride)blends by controlling selective localization and surface modification of SiC nanoparticles[J].ACS Applied Materials&Interfaces,2013,5(15):6915-6924.
[9]Kusunose T,Yagi T,Firoz SH,et al.Fabrication of epoxy/silicon nitride nanowire composites and evaluation of their thermal conductivity[J].Journal of Materials Chemistry A,2013,1(10):3440-3445.
[10]Wu YP,Xue Y,Qin S,et al.BN nanosheet/polymer films with highly anisotropic thermal conductivity for thermal management applications[J].ACSApplied Materials&Interfaces,2017,9(49):43163-43170.
[11]Yao YM,Sun JJ,Zeng XL,et al.Construction of3D skeleton for polymer composites achieving a high thermal conductivity[J].Small,2018,14(13):e1704044.
[12]Zhang J,Wang XN,Yu CP,et al.A facile method to prepare flexible boron nitride/poly(vinyl alcohol)composites with enhanced thermal conductivity[J].Composites Science and Technology,2017,149:41-47.
[13]Li GH,Xing RF,Geng PP,et al.Surface modification of boron nitride via poly(dopamine)coating and preparation of acrylonitrile-butadienestyrene copolymer/boron nitride composites with enhanced thermal conductivity[J].Polymers for Advanced Technologies,2018,29(1):337-346.
[14]Dai XJ,Chen Y,Chen ZQ,et al.Controlled surface modification of boron nitride nanotubes[J].Nanotechnology,2011,22(24):245301.
[15]Yu JH,Huang XY,Wu C,et al.Interfacial modification of boron nitride nanoplatelets for epoxy composites with improved thermal properties[J].Polymer,2012,53(2):471-480.
[16]Terao T,Zhi CY,Bando Y,et al.Alignment of boron nitride nanotubes in polymeric composite films for thermal conductivity improvement[J].Journal of Physical Chemistry C,2010,114(10):4340-4344.
[17]Lin ZY,Liu Y,Raghavan S,et al.Magnetic alignment of hexagonal boron nitride platelets in polymer matrix:toward high performance anisotropic polymer composites for electronic encapsulation[J].ACS Applied Materials&Interfaces,2013,5(15):7633-7640.
[18]Lin ZY,Liu Y,Moon KS,et al.Enhanced thermal transport of hexagonal boron nitride filled polymer composite by magnetic field-assisted alignment[C]//2013 IEEE 63rd Electronic Components and Technology Conference(ECTC),2013:1692-1696.
[19]Zeng XL,Yao YM,Gong ZY,et al.Ice-templated assembly strategy to construct 3D boron nitride nanosheet networks in polymer composites for thermal conductivity improvement[J].Small,2015,11(46):6205-6213.
[20]Huang T,Zeng XL,Yao YM,et al.A novel h-BNRGOhybrids for epoxy resin composites achieving enhanced high thermal conductivity and energy density[J].RSC Advances,2017,7(38):23355-23362.
[21]Huang T,Zeng XL,Yao YM,et al.Boron nitride@graphene oxide hybrids for epoxy composites with enhanced thermal conductivity[J].RSC Advances,2016,6(42):35847-35854.
[22]Gao Y,Zhu PL,Li G,et al.The preparation of SiO2@BN/epoxy composites with high thermal conductivity and excellent thermo-mechanical property[C]//2017 18th International Conference on Electronic Packaging Technology(ICEPT),2017:1300-1303.
[23]Li ZL,Ju DD,Han LJ,et al.Formation of more efficient thermally conductive pathways due to the synergistic effect of boron nitride and alumina in poly(3-hydroxylbutyrate)[J].Thermochimica Acta,2017,652:9-16.
[24]Su JL,Xiao Y,Ren M.Enhanced thermal conductivity in epoxy nanocomposites with hybrid boron nitride nanotubes and nanosheets[J].Physica Status Solidi A,2013,210(12):2699-2705.
[25]Wang FF,Yao YM,Zeng XL,et al.Highly thermally conductive polymer nanocomposites based on boron nitride nanosheets decorated with silver nanoparticles[J].RSC Advances,2016,6(47):41630-41636.
[26]Liu KH,Liu L,Luo YF,et al.One-step synthesis of metal nanoparticle decorated graphene by liquid phase exfoliation[J].Journal of Materials Chemistry,2012,22(38):20342-20352.
[27]Liu KH,Chen SL,Luo YF,et al.Noncovalently functionalized pristine graphene/metal nanoparticle hybrid for conductive composites[J].Composites Science and Technology,2014,94:1-7.
[28]Shen JF,Shi M,Li N,et al.Facile synthesis and application of Ag-chemically converted graphene nanocomposite[J].Nano Research,2010,3(5):339-349.
[29]Solin SA,Nemanich RJ,Martin RM.Lightscattering and X-ray-scattering studies of boronnitride micro-crystals[J].Bulletin of the American Physical Society,1981,26(3):485-485.
[30]Nemanich RJ,Solin SA,Martin RM.Lightscattering study of boron-nitride micro-crystals[J].Physical Review B,1981,23(12):6348-6356.
[31]Hoffman DM,Doll GL,Eklund PC.Opticalproperties of pyrolytic boron-nitride in the energyrange0.05-10 eV[J].Physical Review B,1984,30(10):6051-6056.
[32]Que RH,Huang YC,Li QL,et al.Generating electric current based on the solvent-dependent charging effects of defective boron nitride nanosheets[J].ACS Applied Materials&Interfaces,2014,6(22):19752-19757.
[33]Hou J,Li GH,Yang N,et al.Preparation and characterization of surface modified boron nitride epoxy composites with enhanced thermal conductivity[J].RSC Advances,2014,4(83):44282-44290.
[34]Brosseau C.Generalized effective medium theory and dielectric relaxation in particle-filled polymeric resins[J].Journal of Applied Physics,2002,91(5):3197-3204.
[35]Fang LJ,Wu C,Qian R,et al.Nano-micro structure of functionalized boron nitride and aluminum oxide for epoxy composites with enhanced thermal conductivity and breakdown strength[J].RSCAdvances,2014,4(40):21010-21017.