Citation: Tianqi Bai, Kun Huang, Fachen Liu, Ruochen Shi, Wencai Ren, Songfeng Pei, Peng Gao, Zhongfan Liu. Nanoscale Mechanism of Microstructure-Dependent Thermal Diffusivity in Thick Graphene Sheets[J]. Acta Physico-Chimica Sinica, ;2025, 41(3): 240402. doi: 10.3866/PKU.WHXB202404024 shu

Nanoscale Mechanism of Microstructure-Dependent Thermal Diffusivity in Thick Graphene Sheets

Tianqi Bai ^{1, 2, †} ,
Kun Huang ^{3, 4, †} ,
Fachen Liu ^{1, 2} ,
Ruochen Shi ^{1, 5} ,
Wencai Ren ^{3, 4} ,
Songfeng Pei ^{3, 4,,} ,
Peng Gao ^{1, 2, 5, 6, 7, 8,,} ,
Zhongfan Liu ^{6, 9,,}

1.
Electron Microscopy Laboratory, School of Physics, Peking University, Beijing 100871, China
2.
Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China
3.
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
4.
School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China
5.
International Center for Quantum Materials, Peking University, Beijing 100871, China
6.
Beijing Graphene Institute, Beijing 100095, China
7.
Collaborative Innovation Center of Quantum Matter, Beijing 100871, China
8.
Interdisciplinary Institute of Light-Element Quantum Materials and Research Center for Light-Element Advanced Materials, Peking University, Beijing 100871, China
9.
National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China

Corresponding author: Songfeng Pei, pgao@pku.edu.cn Peng Gao, sfpei@imr.ac.cn Zhongfan Liu, zfliu@pku.edu.cn
Received Date: 17 April 2024
Revised Date: 13 June 2024
Accepted Date: 17 June 2024

Fund Project: the National Natural Science Foundation of China T2188101the National Natural Science Foundation of China 52125307the National Natural Science Foundation of China 52021006the National Natural Science Foundation of China 52273240

The rapid advancement in the integration density of electronic components has led to a pressing need for effective thermal management solutions. Among the promising materials in this regard, graphene stands out due to its exceptional thermal conductivity properties. Currently, the production of ultra-high thermally conductive thick graphene sheets primarily involves the reduction of graphene oxide. However, despite significant progress, the impact of defects on thermal properties remains inadequately understood, limiting the achievement of thermal conductivity exceeding 1500 W·m^-1·K^-1. During the preparation process of reduced graphene oxide-based graphene sheets, hole structures are inevitably formed, reducing the overall density and thus decreasing thermal conductivity. However, the influencing factors on thermal diffusivity, one of the determining factors of thermal conductivity, have not been reported. Thus, we defined the intrinsic thermal diffusivity specific to materials with internal holes and further investigated the correlation between the intrinsic thermal diffusivity of thick graphene sheets and microstructure through various electron microscopy characterization, thermal diffusivity measurements, and simulations. We aim to elucidate the factors and mechanisms affecting the thermal diffusivity and hence thermal conductivity. Our research reveals subtle insights, particularly regarding the impact of holes of different sizes and quantities on thermal diffusivity. Notably, our simulation results show that a real dense-small-holes structure in graphene sheets can reduce thermal diffusivity by 39.4%, more than twice the reduction caused by a single-large-hole structure (16.1%). Statistical conclusions obtained through three-dimensional reconstruction also perfectly match these computational results. We emphasize that the presence of dense-small-holes structures disrupt the original high-speed heat transfer paths more severely, while the effect of single-large-hole structures are relatively weaker, primarily reducing overall density and thus thermal conductivity. Additionally, we found that the out-of-plane crystallinity has a significant impact on thermal diffusivity, further enhancing our understanding of microstructural factors affecting thermal diffusivity. By elucidating these mechanisms, our findings make significant contributions to the technological advancement of producing ultra-high thermally conductive thick graphene sheets. A deeper understanding of the interaction between microstructure and thermal performance brings hope for the development of next-generation electronic device thermal management solutions. Through continued research in this field, we anticipate further improvements in the performance and efficiency of graphene thermal management systems, ultimately driving innovation in electronic device design and manufacturing.
- Thick graphene sheets,
- Intrinsic thermal diffusivity,
- Single large hole,
- Dense small holes,
- Out-of-plane crystallinity
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