A review of three-dimensional graphene networks for use in thermally conductive polymer composites: construction and applications
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摘要: 随着电子设备的耗电量和发热量不断增加，这对于热管理材料的散热性能提出了更高的要求。石墨烯已被广泛用作导热填料以提高聚合物的导热性。然而，石墨烯纳米片在聚合物中的分散性差，极大地限制了其在热管理中的实际应用。构建相互连接的三维石墨烯网络是提高聚合物复合材料的导热性的一个有效策略。本综述总结了最近三维石墨烯基导热聚合物复合材料（3D GPCs）的构建和应用方面的研究进展。此外，还总结了提高3D GPCs导热系数的方法。最后，提出了对于当前3D GPCs的挑战和展望。Abstract: As the power consumption and heat generation of electronic devices continue to increase, higher demands are being placed on thermal management materials for heat dissipation. Graphene has been widely used as a thermally conductive filler to improve the thermal conductivity of polymers. However, the poor dispersibility of graphene nanoplates in polymers dramatically limits their practical use in thermal management. A promising strategy to increase the thermal conductivity of polymer composites is to construct interconnected three-dimensional graphene networks. This review summarizes the recent advances in the construction and applications of three-dimensional graphene-based polymer composites and ways to improve their thermal conductivity. The current challenges and prospects for the preparation and applications of these materials are considered.
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Figure 1. Schematic illustration of various 3D graphene networks for highly thermally conductive polymer composites.
Figure 2. (a) (i) Growth profile of 3D GF by CVD using Ni foam as the template, (ii) Photo image of as-produced free-standing 3D GF film after removal of Ni template by chemical etching and (iii) SEM of free-standing GF[28]. (b) Flowchart for the preparation of graphene foam[29]. (c) Schematic for the synthesis process of GNs/GF/NR composites[30] . (Reproduced with permission).
Figure 3. (a) The preparation process of the GF/epoxy composite[35]. (b) Schematic illustration of (i) fabrication process of the DAGF and (ii) the corresponding structural change of each step based on the proposed dual-assembly method[36]. (c) SEM images of (i) MF, (ii) GO@MF and (iii) reduced GO (RGO)@MF[37]. (d) Illustration of the overall preparation procedures of the polymer nanocomposite[37]. (Reproduced with permission).
Figure 4. (a) Schematic illustration of the fabrication of anisotropic high-quality graphene aerogels[39] and (b) Fabrication and microstructure of 3D BN-rGO/epoxy composites: (i) the fabrication of 3D BN-rGO/epoxy composites, (ii) optical and (iii) cross-sectional SEM images of 3D BN-GO skeleton, (iv) SEM image showing the presence of BN large through-plane connected layers of GO and (v) SEM image of fractured surface of 3D BN-rGO/epoxy composites[40]. (Reproduced with permission).
Figure 5. (a) Diagrams of fabrication procedure for graphitized graphene aerogel (gGA)/silicon rubber (SR)[41]. (b) Simulation schematic of the thermal conductive path in PBGF composites[42]. (c) Preparation and structure of graphene/PBONF[49]. (d) Schematic illustration of the overall fabrication procedure of rGO-BN-NR film[45]. (e) (i) Cross-section SEM images of gGA[41], SEM image of (ii) GF, (iii) BGF[42]and (iv) freezing dried hydrogel, showing a 3D PBONF network with homogeneously distributed GNS[49]and (v) SEM microstructure image of the dried gel of rGO-BN[45]. (Reproduced with permission).
Figure 6. (a) Devices fabrication process. (b) Printing devices using hybrid ink[52]. (c) SEM images of PS/GNP composite particles[56]. (d) Schematic illustration of preparation of the PS/GO-PDA composites under high pressure with a continuous three-dimensional network (Inset: photograph of the PS/GO-PDA thin film[57]) . (e) Preparation procedures of (PS/MWCNT)@GNP nanocomposites with the segregated double network[58]. (Reproduced with permission).
Figure 8. (a) Fabrication process of MGW and MGW/epoxy nanocomposites[65]. (b) (i) Schematic illustrating the fabrication of anisotropically conductive epoxy composite, top-view SEM images of (ii) fGHF5, (iii) fGF, (iv) GHF5 and (v) GM. Digital images of hydrogels and corresponding foams dried under ambient conditions with different GO/GNP mass ratios of (vi) 1/0 and (vii) 1/5[68]. (c) (i, iii, v) Top-view and (ii, iv, vi) side-view SEM images of TAGA-2800 prepared by using three directional freezing rates: (i, ii) floating the copper disk on liquid nitrogen, (iii, iv) putting the disk on a copper cylinder that is dipped in liquid nitrogen, and (v, vi) hanging the disk above the liquid nitrogen and (vii) epoxy/TAGA1.5-2800 with different directional-freezing rates[63]. (Reproduced with permission).
Figure 9. (a) (i) Schematic configuration of the TIM performance test system and the heat flow diffusion path along the vertical direction. (ii) The photograph and the cross-sectional SEM image of the DAGF5/PDMS composites. (iii) The heater temperature evolution versus the running time at the power density of 50 W cm−2. (iv) Thermal shock stability in cyclic heating/cooling tests and (v) thermal durability in a long-term TIM performance test (10 days) using DAGF5/PDMS as a TIM[36]. (b) (i) Demonstration of PP/PDA/G composite as a thermal management material for heat dissipation of a LED lamp, (ii) The surface temperature variations of LED versus time, (iii) Comparison of infrared thermal images of LED integrated with PP/PDA/G and pure PP as thermal management materials[80]. (c) (i) Photograph of the in-situ test system, (ii) Profiles of the surface temperature-time of a ceramic heater at 4 V with fan cooling (insets are IR images of the c-GF/PDA/APTS/PDMS composite), (iii) Breakdown strength and (iv) electrical resistivity of studied materials[79], (d) Visible light images and the corresponding IR images of CPUs integrated with self-made heat sinks[82]. (Reproduced with permission).
Figure 10. (a) Thermal energy storage and release: (i) Experimental setup for light-to-heat conversion, (ii) Schematic diagram of light-to-heat conversion and storage, (iii) Temperature evolution curves of pure PEG and composite PCMs and (iv) θ of the composite PCMs[86]. (b) Shape-stability with increasing temperature[86]. (c) (i-iii) The images of flexible GAF-PW CPCF, infrared imaging pictures of human model with GAF-PW CPCF coated on the one side of arm and chest (iv) under the irradiation for 210 s and (v) after removing the irradiation for 10 s[88]. (Reproduced with permission).
Table 1. Summary on thermal conductivities of polymer composites filled with 3D graphene prepared by different methods.
Sample TC of matrix
(W m−1 K−1)TC of composites
(W m−1 K−1)Loading
(%)TC enhancement
efficiency (η)Density
(g/cm3)Method Testing
MethodRefs. 3DGF/EP 0.1898 0.52 0.27 644.0 CVD LFA [29] GNs/GF/NR 0.13 10.64 6.2%(vol.) CVD LFA [30] MGW/EP(||) 0.2 8.8 8.3 518.0 0.096 CVD LFA [65] GF/PDA/APTS/PDMS(⊥) 0.18 1.62 11.62 69.0 1.31 CVD LFA [79] GF/PDA/APTS/PDMS(||) 28.77 1367.0 GF/h-Fe3O4/PDMS(||) 0.18 28.12 12 1300.0 0.017 CVD LFA [92] GF/h-Fe3O4/PDMS(⊥) 2.42 103.7 GF/EP 0.1758 8.04 6.8 657.8 Polymer template LFA [35] DAGF/EP(||) 0.2 24.8 13.3%(vol.) 0.27 Polymer template LFA [36] DAGF/EP(⊥) 62.4 RGO/MF/PDMS 0.175 2.19 4.82 238.9 1.89 Polymer template Hot Disk [37] c-GA/MF/PEG 0.32 1.32 4.6 67.9 0.022 Polymer template Hot Disk [87] AGAs/PW(||) 0.35 2.68 8 mg/mL 0.025 Ice template LFA [39] AGAs/PW(⊥) 8.87 BN-rGO/EP(⊥) 0.18 5.05 13.16%(vol.) Ice template LFA [40] TAGA/EP(⊥) 0.17 6.57 1.5 2509.8 Ice template LFA [63] TAGA/EP(||) 1.15 384.3 PEG/HGA 0.31 1.43 2.25 160.6 Ice template Hot Disk [86] VAIGN/EP(⊥) 0.16 2.13 0.92%(vol.) 1.27 Ice template LFA [93] gGA/SR 0.23 1.26 0.5 895.65 Self-assembly Hot Disk [41] 3D BNNS/GF/PA6 0.196 0.891 8.4 42.21 1.081 Self-assembly LFA [42] rGO/BN/NR(||) 16 260phr 1.57 Self-assembly LFA [45] GNS/PBONF 13.2 133 70 13.0 1.5 Self-assembly LFA [49] 3D BNNT/GONS/EP 0.23 4.53 11.6%(vol.) Self-assembly Steady-state [50] (f)SiC/GO/EP 0.22 0.91 30 10.45 Self-assembly Hot Disk [51] GNP/RGO/octadecanol 0.23 5.92 12 206.2 0.21 Self-assembly LFA [67] GHF/EP(||) 0.21 3.22 35 41 0.42 Self-assembly LFA [68] GHF/EP(⊥) 8.43 111.8 GNP/RGO/octadecanol 0.21 9.5 13.3 332.6 0.09 Self-assembly LFA [84] RGO/BN/EP 0.15 11.01 44 164.5 1.61 Self-assembly LFA [94] CF/GNP/EP 0.2 2 16.9 53.3 1.24 3D printing LFA [52] rGO/GNP/PDMS 0.186 3 18.1 83.6 1.1 Foaming method LFA [53] Graphene microspheres/EP 0.26 0.96 1 437.0 Liquid nitrogen driven assembly Hot Disk [54] GO/PDA/PS(||) 0.23 4.13 0.96%(vol.) Hot pressing LFA [57] GO/PDA/PS(⊥) 4.56 PS/GNP/MWCNT 0.18 1.08 5 %(vol.) Hot pressing Hot Disk [58] RGO/TPU 0.1818 0.8 1.04 327.0 Hot pressing LFA [95] Note: enhancement efficiency: $\eta = \dfrac{ {TC - T{C_0} } }{ {100WT{C_0} } } \times 100$, Where η is TC enhancement efficiency, TC and TC0 are TC of composite and pure polymer, respectively. W is the weight loading of fillers. 
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