Preparation and properties of AlN/Si3N4/PI composites
WU Yunxiang1,2, LEI Ting1, GAO Jiming2, YANG Yang3
1. State Key Laboratory of Powder Metallurgy, Changsha 410083, China; 2. Zhuzhou Times New Material Technology Co., Ltd., Zhuzhou 412007, China; 3. Jones Technology (Wuxi) Co., Ltd., Wuxi 214028, China
Abstract：High thermal conductivity polyimide composites have good development prospects in integrated electronic circuits, aerospace and other fields because of their good comprehensive properties. In this paper, silicon nitride whiskers and aluminum nitride particles with high thermal conductivity were selected as inorganic fillers, and surface modification was made with titanate coupling agent, and silicon nitride whiskers/aluminum nitride particles/polyimide (AlN/Si3N4/PI) composite films were synthesized in situ. The structure and properties of the composite films were characterized by scanning electron microscopy (SEM), Hot Disk tester and tensile tester. The results show that when the volume ratio of AlN/Si3N4 is 4:2, the composite filler forms a good thermal conductivity network in the matrix. When the total filler volume fraction reaches 30%, the thermal conductivity of the composite film reaches the maximum of 0.84 W/(m·K). The mechanical properties of the composites decrease with the increase of filler content, and the heat resistance increases with the increase of filler content.
[1] WANG H T, DING D L, LIU Q, et al.Highly anisotropic thermally conductive polyimide composites via the alignment of boron nitride platelets[J]. Composites Part B: Engineering, 2019, 158: 311-318 [2] YUAN R, JU P, WU Y, et al.Silane-grafted graphene oxide improves wear and corrosion resistance of polyimide matrix: Molecular dynamics simulation and experimental analysis[J]. Journal of Materials Science, 2019, 54(27): 11069-11083. [3] LIAW D J, WANG K L, HUANG Y C, et al.Advanced polyimide materials: Syntheses, physical properties and applications[J]. Progress in Polymer Science, 2012, 37(7): 907-974. [4] TIPTIPAKORN S, KUENGPUTPONG N, OKHAWILAI M, et al.Improvement of polyimide/polysulfone composites filled with conductive carbon black as positive temperature coefficient materials[J]. Journal of Applied Polymer Science, 2019, 173(12): 48482. [5] GUO Y Q, LYU Z Y, YANG X T, et al.Enhanced thermal conductivities and decreased thermal resistances of functionalized boron nitride/polyimide composites[J]. Composites Part B: Engineering, 2019, 164: 732-739. [6] LI J W, DING Y Q, GAO Q, et al.Ultrathin and flexible biomass-derived C@CoFe nanocomposite films for efficient electromagnetic interference shielding[J]. Composites Part B: Engineering, 2020, 190:107935. [7] ZHANG Y, HEO Y J, SON Y R, et al.Recent advanced thermal interfacial materials: A review of conducting mechanisms and parameters of carbon materials[J]. Carbon, 2019, 142: 445-460. [8] MA X, LIU L, HE H, et al.Effects of interface bonding on the corona resistance of the polyimide/nano-Al2O3 three-layer composite films[J]. High Performance Polymers, 2018, 30(10): 1240-1246. [9] LI X, XU J L, JIANG Y D, et al.Toward agricultural ammonia volatilization monitoring: A flexible polyaniline/Ti3C2Tx hybrid sensitive films based gas sensor[J]. Sensors and Actuators: B. Chemical, 2020, 316: 128144. [10] MA L, WANG Y, XU X, et al.Structural evolution and thermal conductivity of flexible graphite films prepared by carboxylic graphene/polyimide[J]. Ceramics International, 2020, 47(1): 1076-1085. [11] DING D, SHANG Z, ZHANG X, et al.Greatly enhanced thermal conductivity of polyimide composites by polydopamine modification and the 2D-aligned structure[J]. Ceramics International, 2020, 46(18): 28363-28372. [12] LI R, LÜ X, YU J, et al.Dielectric, thermally conductive, and heat-resistant polyimide composite film filled with silver nanoparticle-modified hexagonal boron nitride[J]. High Performance Polymers, 2020, 32(10): 1181-1190. [13] CAO L, WANG J J, DONG J, et al.Preparation of highly thermally conductive and electrically insulating PI/BNNSs nanocomposites by hot-pressing self-assembled PI/BNNSs microspheres[J]. Composites Part B: Engineering, 2020, 188: 107882. [14] LIU L Z, CAO C H, MA X Y, et al.Thermal conductivity of polyimide/AlN and polyimide/(AlN+BN) composite films prepared by in-situ polymerization[J]. Journal of Macromolecular Science, Part A, 2020, 57(5): 398-407. [15] HE X H, YU X, WANG Y C.Significantly enhanced thermal conductivity in polyimide composites with the matching of graphene flakes and aluminum nitride by in situ polymerization[J]. Polymer Composites, 2020, 41(2): 740-747. [16] DUAN G Y, CAO Y T, QUAN J Y, et al.Bioinspired construction of BN@polydopamine@Al2O3fillers for preparation of a polyimide dielectric composite with enhanced thermal conductivity and breakdown strength[J]. Journal of Materials Science, 2020, 55(19): 8170-8184. [17] TOMINAGA Y, SATO K, HOTTA Y, et al.Effect of the addition of Al2O3 and h-BN fillers on the thermal conductivity of a cellulose nanofiber/nanodiamond composite film[J]. Cellulose, 2019, 26(9): 5281-5289. [18] LUO J B, WU Y P, SUN Y, et al.Preparation and characterization of high thermal conductivity and low cte polyimide composite reinforced with diamond nanoparticles/SiC Whiskers for 3D IC interposer RDL dielectric[J]. Applied Sciences, 2019, 9(9): 1962-1975. [19] DAI W, YU J H, LIU Z D, et al.Enhanced thermal conductivity and retained electrical insulation for polyimide composites with SiC nanowires grown on graphene hybrid fillers[J]. Composites Part A, 2015, 76: 73-81. [20] CHEN M H, ZHOU W Q, ZHANG J W, et al.Dielectric property and space charge behavior of polyimide/silicon nitride nanocomposite films[J]. Polymers, 2020, 12(2): 322-333. [21] YANG M, ZHANG C H, SU G D, et al.Preparation and wear resistance properties of thermosetting polyimide composites containing solid lubricant fillers[J]. Materials Chemistry and Physics, 2020, 241:122034. [22] YANG X, YU X, Naito K, et al.Enhanced thermal conductivity of polyimide composites filled with modified h-BN and nanodiamond hybrid filler[J]. Journal of Nanoscience and Nanotechnology, 2018, 18(5): 3291-3298. [23] YANG Y, GAO J, LEI T, et al.Thermal conductivity and mechanical properties of polyimide composites with mixed fillers of BN flakes and SiC@SiO2whiskers[J]. Polymer Engineering & Science, 2020, 60(5): 1044-1053.
2021, Vol. 26 
