Research progress of carbon-based fillers in polymer matrix insulating and thermally conductive composites
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摘要: 集成电路产业的高质量发展对其产业链中配套材料的绝缘导热性能提出了更高的要求。具有高导热、低密度、活性表界面等优异特性的碳系材料在聚合物基复合材料中的基础研究，对于高性能绝缘导热材料的性能提升及应用发展至关重要。基于此，本文系统地综述了聚合物基绝缘导热复合材料中碳系填料的研究进展。首先，介绍了聚合物基复合材料的导热机制、绝缘机制及绝缘导热兼容机制。其次，对碳系填料的表面处理和空间结构及分布控制方法进行了综述，研究其绝缘导热性能控制机制。最后，对聚合物基绝缘导热复合材料研究工作中尚未解决的科学问题、技术难点及未来发展方向进行了总结和展望。Abstract: The high-quality development of the integrated circuit industry puts forward higher requirements for the insulation properties and thermal conductivity of supporting materials in its industrial chain. The basic research of carbon-based materials with excellent properties, such as high thermal conductivity, low density and active surface interface in polymer matrix composites, is essential for the performance improvement and application development of high-performance insulating and thermally conductive materials. This article systematically reviews the research progress of carbon-based fillers in polymer matrix insulating and thermally conductive composites. Firstly, the thermal conduction mechanism, insulation mechanism, and insulation and thermal conduction compatibility mechanism of polymer matrix composites were introduced. Secondly, the surface treatment, spatial structure and distribution control methods of carbon-based fillers were reviewed, and the control mechanism of insulation properties and thermal conductivity wass studied. Finally, the unresolved scientific problems, technical difficulties and future development directions in the research work of polymer matrix insulating and thermally conductive composites were summarized and prospected.
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Key words:
- carbon-based fillers /
- thermal conductivity /
- electrical insulation /
- polymer matrix /
- composites
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图 1 聚多巴胺封装还原氧化石墨烯(PDA@rGO)的制备示意图 (a)、三维互连石墨烯网络的PDA@rGO/硅橡胶(SR)复合材料的制备过程示意图 (b)[15]
Figure 1. Schematic illustration of the preparation of polydopamine-coated reduced graphene oxide (PDA@rGO) (a) , schematic illustration of the preparation process of the PDA@rGO/silicone rubber (SR) composite with 3D interconnected graphene networks (b)[15]
图 2 在石墨烯纳米片(GNP)上形成纳米SiO2涂层的示意图 (a)、GNP/聚二甲基硅氧烷(PDMS)和SiO2@GNP/PDMS复合材料中热和电子传输途径的示意图 (b)[17]
Figure 2. Schematic illustration of formation of nano SiO2 coating onto graphene nanoplatelet (GNP) (a) , schematic mechanism for formation of heat and electron transport pathways in the GNP/polydimethylsiloxane (PDMS) and SiO2@GNP/PDMS composites (b)[17]
CTAB—Cetyltrimethyl ammonium bromide; TEOS—Tetraethyl orthosilicate
表 1 部分聚合物基复合材料的绝缘导热性能及其控制机制
Table 1. Electrical insulation properties and thermal conductivity and its control mechanism of some polymer matrix composites
Sample Fraction Thermal conductivity/
(W·m−1·K−1)Electrical insulation properties Control mechanism PDA@CuNW-PDA@GO/EP[14] 2wt% 0.4 >1.2×1014 Ω·cm Polymer encapsulation PDA@rGO/SR[15] 1.5wt% 1.5 >1013 Ω·cm Polymer encapsulation MgO@CF/PA6[16] 20wt% 0.7 — Ceramic coating treatment SiO2@GNP/PDMS[17] 2wt% 0.5 9.2×1012 Ω·cm Ceramic coating treatment Al2O3@GNP/EP[23] 12wt% 1.5 6.7×10−9 S/m Ceramic coating treatment FCNT/NFC[24] 35wt% 14.1 >1010 Ω·cm Fluorination modification PMMA-g-FCNT/PMMA[25] 15wt% 1.2 >1013 Ω·cm Fluorination modification GFS/PVA[27] 93wt% 61.3 >1011 Ω·cm Fluorination modification BNNS-CNT/Cellulose[28] 15wt% 11.8 >1010 Ω·cm Micro-hybrid structure control CNT-NH2-Fe@h-BN/CER[29] 32wt% 0.9 <1.2×10−12 S/cm Micro-hybrid structure control BNNT-GONS/EP[30] 11.6vol% 4.5 55 kV/mm Micro-hybrid structure control h-BN-NfG/CER[31] 30wt% 3.4 6.1×10−12 S/cm Micro-hybrid structure control h-BN-mG/CER[32] 35wt% 1.3 <1.5×10−10 S/cm Micro-hybrid structure control BN-GS/EP[33] 15.9wt% 0.6 3.0×10−7 S/cm Micro-hybrid structure control AlN-BN/PP-AlN-MWCNT/PP[37] 70wt% 3.4 6.6×1013 Ω·cm Macro-layered structure control BN/SR-GNP/SR[38] 17.9vol% 8.5 ~1012 Ω·cm Macro-layered structure control Gt-MWCNT/HDPE-BN/HDPE[40] 32.6vol% 1.5 5×1013 Ω·cm Macro-layered structure control CF-BN/PS-PP[43] 32.5wt% 0.6 — Controllable selective distribution CNT-Pglass/BN-PP[44] 12.5wt% 0.9 ~6×10−5 S/m Controllable selective distribution h-BN-GNP/PA6[45] 18.8vol% 2.7 4.1×10−9 S/m Controllable selective distribution Notes: @—Coating relationship; PDA—Polydopamine; CuNW— Cu nanowire;GO—Graphene oxide; EP—Epoxy resin; SR—Silicone rubber; rGO—Reduced graphene oxide; PMMA—Polymethyl methacrylate; PDMS—Polydimethylsiloxane; Gt—Graphite; NFC—Nanofibrillated cellulose; CF—Carbon fiber; PS—Polystyrene; PP— Polypropylene; MWCNT—Multiwalled carbon nanotube; GNP—Graphene nanosheets; GONS—Graphene oxide nanosheets; BNNT—Boron nitride nanotube; HDPE—High-density polyethylene; CNT—Carbon nanotube; mG—Multilayer graphene; BNNS—BN nanosheets; NfG—Amino functionalized graphene; FCNT—Fluorinated carbon nanotubes; GS—Graphene sponge; PVA—Polyvinyl alcohol; Pglass—Phosphate glass; GFS—Fossilized fluoroalkene; PA6—Polyamide 6. 
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