石墨烯导热研究进展

doi:10.3866/PKU.WHXB202101013

物理化学学报 >> 2022, Vol. 38 >> Issue (1): 2101013.doi: 10.3866/PKU.WHXB202101013

所属专题：石墨烯的功能与应用

石墨烯导热研究进展

宋厚甫¹, 康飞宇¹^,²^,³^,*()

¹ 清华大学，清华-伯克利深圳学院，广东深圳 518055
² 清华大学深圳国际研究生院，广东省热管理工程与材料重点实验室，广东深圳 518055
³ 清华大学深圳国际研究生院，深圳盖姆石墨烯研究中心，广东深圳 518055

收稿日期:2021-01-07 录用日期:2021-02-08 发布日期:2021-02-25
通讯作者: 康飞宇 E-mail:fykang@sz.tsinghua.edu.cn
作者简介:康飞宇，1962年出生。获香港科技大学博士学位; 现任清华大学深圳国际研究生院副院长，清华大学教授、博士生导师。主要研究方向为新型碳材料的制备、表征和应用，特别是石墨、石墨烯及其在锂离子电池与其它储能器件中的应用
基金资助:
广东省科技计划项目(2020B1212060015)及深圳盖姆石墨烯研究中心资助

Recent Progress on Thermal Conduction of Graphene

Houfu Song¹, Feiyu Kang¹^,²^,³^,*()

¹ Tsinghua-Berkeley Shenzhen Institute (TBSI), Tsinghua University, Shenzhen 518055, Guangdong Province, China
² Tsinghua Shenzhen International Graduate School, and Guangdong Provincial Key Laboratory of Thermal Management Engineering & Materials, Shenzhen 518055, Guangdong Province, China
³ Shenzhen Geim Graphene Research Center, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, Guangdong Province, China

Received:2021-01-07 Accepted:2021-02-08 Published:2021-02-25
Contact: Feiyu Kang E-mail:fykang@sz.tsinghua.edu.cn
About author:Feiyu Kang. Email: fykang@sz.tsinghua.edu.cn
Supported by:
广东省科技计划项目(2020B1212060015)及深圳盖姆石墨烯研究中心资助

摘要/Abstract

摘要：

石墨烯具有目前已知材料中最高的热导率，在电子器件、信息技术、国防军工等领域具有良好的应用前景。石墨烯导热的理论和实验研究具有重要意义，在最近十年间取得了长足的发展。本文综述了石墨烯本征热导率的研究进展及应用现状。首先介绍应用于石墨烯热导率测量的微纳尺度传热技术，包括拉曼光谱法、悬空热桥法和时域热反射法。然后展示了石墨烯热导率的理论研究成果，并总结了石墨烯本征热导率的影响因素。随后介绍石墨烯在导热材料中的应用，包括高导热石墨烯膜、石墨烯纤维及石墨烯在热界面材料中的应用。最后对石墨烯导热研究的成果进行总结，提出目前石墨烯热传导研究中存在的机遇与挑战，并展望未来可能的发展方向。

关键词: 石墨烯, 热导率, 声子, 热界面材料, 悬空热桥法, 尺寸效应

Abstract:

With the irreversible trend of miniaturization and the pursuit of a high power density in electronic devices, heat dissipation has become crucial for designing next-generation electronic products. Graphene, which has the highest thermal conductivity among all discovered solid materials, has attracted attention from both academia and the industry. As a two-dimensional material with atom-scale thickness, graphene is suitable for investigating the phonon transport behavior at reduced dimensions. The mass production technique of graphene makes it a promising material for thermal management in consumer electronics, information technology, medical devices, and new energy automobiles. In this review, we summarize the recent progress on the thermal conduction of graphene. In the first part, we introduce the thermal conductivity measurement methods for graphene, including the optothermal Raman method, suspended-pad method, and time-domain thermoreflectance (TDTR) method. The thermal measurement of graphene with high accuracy is key to understanding the heat transfer mechanism of graphene; however, it is still a significant challenge. Despite the development of measurement methods, the thermal measurement of suspended single-layer graphene is limited by the graphene transfer technique, estimation of the thermal contact resistance, sensitivity to the in-plane thermal conductivity in the thermal model, and other factors. In the second part, we discuss the theoretical study of the thermal conductivity of graphene via first principle calculations and molecular dynamics simulation. The "selection rule" of phonon scattering explains the thickness-dependent thermal conductivity of few-layer graphene, and the understanding of the contribution of phonon modes to the thermal conductivity of graphene has been updated recently by taking multiple-phonon scattering into consideration. The size effect on the thermal conductivity of graphene is discussed in this section for a better understanding of the phonon transport behavior of graphene. In the third part, we conclude with the thermal management applications of graphene, including a highly thermally conductive graphene film, graphene fiber, and graphene-enhanced thermal interface materials. For graphene films, which are the pioneering thermal management applications in industrial use, we focus on the challenge of fabricating highly thermally conductive graphene films with large thicknesses and propose possible technical methods. For graphene-enhanced thermal interface materials, we summarize the main factors affecting the thermal properties and discuss the tradeoff between the high thermal conductivity of graphene flakes and the dispersibility of graphene in the polymer matrix. It was demonstrated that a 3D thermal conductive network is essential for efficient heat dissipation in graphene-based composites. Finally, a summary of opportunities and challenges in the thermal study of graphene is presented at the end of the review. Research on the thermal properties of graphene has made immense progress since the discovery of the thermal conductivity of graphene more than a decade ago, and will continue in order to address the urgent requirements of thermal management.

Key words: Graphene, Thermal conductivity, Phonon, Thermal interface material, Suspended pad, Size effect

宋厚甫, 康飞宇. 石墨烯导热研究进展[J]. 物理化学学报, 2022, 38(1), 2101013. doi: 10.3866/PKU.WHXB202101013

Houfu Song, Feiyu Kang. Recent Progress on Thermal Conduction of Graphene[J]. Acta Phys. -Chim. Sin. 2022, 38(1), 2101013. doi: 10.3866/PKU.WHXB202101013

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202101013

https://www.whxb.pku.edu.cn/CN/Y2022/V38/I1/2101013

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Sample	Thermal conductivity (W·m^-1·K^-1)	Measurement method	Preparation method
Suspended
Single-layer graphene ⁶	5300 ± 480	Raman	Mechanical exfoliation
Single-layer graphene ¹⁷	2500 + 1100/-1050	Raman	CVD
2-layer graphene ²⁵	620 ± 80	Suspended-pad	Mechanical exfoliation
Single-layer graphene ²⁶	1689 ± 100	Suspended-pad	CVD
Supported
Single-layer graphene ⁸	579 ± 34	Suspended-pad	Mechanical exfoliation, SiO₂ substrate
Single-layer graphene ¹⁶	630	Raman	Mechanical exfoliation, SiO₂ substrate
Single-layer graphene ¹⁷	370 + 650/-320	Raman	CVD, Au/SiNx substrate
3-layer graphene ²⁴	327	Suspended-pad	Mechanical exfoliation, SiNx substrate
Bulk
Multi-layer graphene ³⁵	1930 ± 1400	TDTR	Mechanical exfoliation, thickness 194 nm
HOPG ³⁸	1800	TDTR	Bulk
HOPG ³⁹	1861 ± 744	TDTR	Bulk
HOPG ⁴⁰	1843	TDTR	Bulk
Graphene film ⁴⁸	1100	Laser flash	Reduced graphene oxide
Graphene film ¹⁰	1940	Laser flash	Reduced graphene oxide

Material	Thermal conductivity/(W·m^-1·K^-1)	Preparation method
GO ⁹	2025	Doctor-blade, 3000 ℃ annealing reduction +3000 ℃ second annealing reduction
GO ¹⁰	1940	Casting, 3000 ℃ annealing reduction
GO ⁴⁸	1100	Evaporation, 2000 ℃ annealing reduction
GO ⁷⁶	1283–1434	Electro-spray deposition，2850 ℃ annealing reduction
GO ⁷⁷	1390	Vacuum filtration, HI reduction
Graphene ⁷⁸	1529	Ball milling，2850 ℃ annealing reduction
GO ⁸¹	1224	Doctor-blade, film paste Hot pressing + 2800 ℃ annealing reduction

Fillers	Loading	Thermal conductivity/(W·m^-1·K^-1)	Method
rGO ⁹⁶	25% (x)	6.4	Mixing
rGO ⁹⁷	20% (w)	5.8	Silane functionalized
Graphene ⁹⁸	10% (x)	5.1	Sodium cholate functionalized
rGO ¹⁰⁴	5% (w)	1.1	[polyimide] NH₂-functionalized, in situ polymerization
Expanded graphite ¹⁰⁵	25% (w)	3.8	Silane functionalized
rGO ¹⁰⁷	4% (w)	1.9	Pyrene derivatives functionalized
Graphene + CNT ¹⁰⁸	20% (x) + 20% (x)	6.3	GNP, multi-walled carbon nanotube
GO ¹¹⁰	10% (w)	0.2	Hot pressed
Graphene 3D network ¹¹	1.23% (x)	3.2	[Wax] CVD grown, annealed
Graphene + CNT 3D network ¹¹⁷	15.8% (x) (in total)	4.1	[Erythritol] CVD grown, annealed

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石墨烯导热研究进展

Recent Progress on Thermal Conduction of Graphene

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