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摘要: 热量累积问题是当前电子产品升级需要解决的首要问题，迫切需要具有优异散热性能的高性能热界面材料。基于热界面材料的发展现状，具有超薄和高垂直热导率的石墨烯纸显示出巨大的潜力。从这个角度，我们介绍了石墨烯/聚合物复合纸、石墨烯/金属复合纸、石墨烯/陶瓷复合纸和石墨烯/碳材料复合纸四种类型杂化石墨烯纸以及垂直排列的石墨烯纸结构。从热界面材料的应用角度，讨论了不同石墨烯纸的优点和局限性，提出了进一步的研究前景，以促进石墨烯纸基热界面材料的实际应用。Abstract: Accumulated heat is the primary problem that needs to be solved in current electronic products. There is an urgent need for designing innovative high-performance thermal interface materials (TIMs) with excellent heat dissipation performance. Based on the development status of TIMs, graphene paper-based TIMs that are ultrathin thickness and have high through-plane thermal conductivity show great potential. From this perspective, we introduce four types of graphene paper (including graphene/polymer composite papers, graphene/metal composite papers, graphene/ceramic composite paper, and graphene/carbon composite paper) and vertically aligned graphene paper as TIMs. Based on the applications of these TIMs, their advantages and limitations are discussed. Finally further research prospects are proposed to promote the practical applications of graphene paper-based TIMs.
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Figure 1. (a) Schematic diagram of a typical ball grid array electronic package (b) Schematic diagram of a TIM filling the air gap between the heater and mating interface of the heat sink. Reprinted with permission from: (a, b) Reference[3], Copyright 2018, MDPI.
Figure 2. Manufacturing method and corresponding structure of the polymer to improve the through-plane thermal conductivity of graphene paper: (a) natural rubber, (b) P(VBcoVA-co-VAc), and (c) polydopamine. Reprinted with permission from: (a) Reference[30], Copyright 2019, American Chemical Society; (b) Reference[31], Copyright 2019, Elsevier; and (c) Reference[33], Copyright 2018, Royal Society of Chemistry.
Figure 4. (a) Schematic of the fabrication process and photograph of silicon carbide/graphene hybrid paper, (b) Morphology and through-plane thermal conductivity of graphene hybrid paper with different thermally conductive structures. Reprinted with permission from: (a) Reference[13], Copyright 2019, American Chemical Society and (b) Reference[43], Copyright 2020, Elsevier.
Figure 5. (a) Schematic assembly of the hierarchical chiral architecture of the graphene-based composite film, (b) Pillared-graphene-CNTs network structure model, (c) Molecular structure of the optimized junction of carbon nanorings and graphene sheets, (d) Schematic illustrating the fabrication process of hierarchically structured graphene paper. Reprinted with permission from: (a) Reference[47], Copyright 2018, American Chemical Society; (b) Reference[48], Copyright 2008, American Chemical Society; (c) Reference[49], Copyright 2018, American Chemical Society and (d) Reference[50], Copyright 2021, Elsevier.
Figure 6. (a) Schematic illustrating the assembly of vertically aligned graphene monolith via “rotating-reassembling” as-prepared graphene paper, (b) Schematic of the fabrication procedure of the vertically aligned graphene paper/PDMS composite, (c) Schematic illustrating the fabrication process of vertically aligned graphene framework, (d) Schematic illustrating the structural change of the graphene based on the proposed method. Reprinted with permission from: (a) Reference[51], Copyright 2011, American Chemical Society; (b) Reference[52], Copyright 2016, Elsevier; (c) Reference[7], Copyright 2021, Elsevier and (d) Reference[4], Copyright 2019, American Chemical Society.
Table 1. The summary of through-plane thermal conductivity with reported graphene-based papers prepared using various methods.
Interlayers/Processing Through-plane thermal conductivity
(W m−1 K−1)Rcontact
(K mm2 W−1)Method Refs. Polymer Nature rubber 0.6 Casting-drying [30] Epoxy 0.8 Directional freezing [32] Naphthalenesulfonate 0.6 Layer-by-layer stacking [53] Cellulose nanofiber 5.0 Filtration [33] PVDF 0.7 Solution casting [54] Metal Au nanoparticles 1.6 In-situ growth [29] Ag nanoparticles 3.3 Casting-drying [34] rGO/AgNW composites 2.6 Hydrothermal [35] Copper particles 5.7 Hot-pressing [36] Ceramic particles BN nanotubes 3.1 Hot-pressing [55] SiC nanowires 17.6 47 In-situ growth [13] SiC nanowires 0.2 Surface functionalization [42] Al2O3 9.1 Hot-pressing [43] Low-dimensional carbon materials Carbon fiber 0.4 Hot-pressing [45] Cellulose nanocrystals 4.6 Evaporation [47] Carbon nanoring 5.8 CVD growth [49] Nanodiamond 0.3 Filtration [44] CNTs 0.1 Hot-pressing [56] CNTs 0.2 Filtration [57] Carbon spheres 1.3 Hydro-thermal [58] Carbon fiber 8.0 [59] Graphene 12.6 Filtration [50] Vertically aligned graphene paper Stacking 75.5 5.1 Coating [51] Rolling with PDMS 614.85 Coating [52] Rolling with PU 276 41 Coating [7] Wrinkling 143 5.8 Filtration [4] 
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