Molecular dynamics simulation of thermal conductivity of diamond/epoxy resin composites

Liu Xiu-Cheng; Yang Zhi; Guo Hao; Chen Ying; Luo Xiang-Long; Chen Jian-Yong

doi:10.7498/aps.72.20222270

Abstract

Improving the thermal conductivity (TC) of epoxy resin thermal interface material is of great significance in tackling the heat dissipation problem of high heat flux in microelectronic chips such as 5G. Using non-equilibrium molecular dynamics (MD) method, the effects of two different filling styles of nano-diamond fillers on the TC of EP based composites are investigated. The results show that the TC of the composite increases with the diamond size when single-particle filling is used, and that a larger diamond size leads to a more significant reduction of the free volume fraction and thus an improvement of the TC. In the multi-particle packing, the composite TC first increases and then decreases with increasing particle number. Increasing the number of particles reduces the free volume fraction, but also results in a larger specific surface area and interfacial thermal resistance, which has a more significant weakening effect on the TC. Moreover, within the same mass fraction of nano-diamond filler, increasing the filler size has a more significant TC improvement on the composite than increasing the number of particles. This study is instructive for the design and preparation of high thermal conductivity nanodiamond/epoxy resin composites.

Keywords:

Authors and contacts

1.
School of Material and Energy, Guangdong University of Technology, Guangzhou 510006, China
2.
Key Laboratory of Cryogenics, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Yang Zhi, yangzhi@gdut.edu.cn

Funds: Project supported by the Joint Funds of the National Natural Science Foundation of China (Grant No. U20A20299).

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References

[1]	Singha S, Thomas M J 2008 IEEE Trans. Dielectr. Electr. Insul. 15 2 Google Scholar
[2]	Li M, Zhou H, Zhang Y, Liao Y, Zhou H 2018 Carbon 130 295 Google Scholar
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图 1 (a) DGEBF, DETDA和金刚石颗粒的分子结构; (b) 计算流程图; (c) 交联反应流程图; (d) 非晶模型; (e) 交联模型

Figure 1. (a) Molecular structures of DGEBF, DETDA and diamond particle; (b) calculation flow charts; (c) process of crosslinking reaction; (d) amorphous model; (e) crosslinked model.

DownLoad: Full-Size Img PowerPoint

图 2 (a) 热传导方向示意图; (b) 冷热端的能量变化; (c) 环氧树脂在x方向上的温度分布

Figure 2. (a) Schematic diagram of heat conduction direction; (b) energy change in hot and cold regions; (c) temperature distribution in the x direction of the epoxy resin.

DownLoad: Full-Size Img PowerPoint

图 3 不同交联率的模型结构　(a) 0%; (b) 32.81%; (c) 64.06%; (d) 90.00%

Figure 3. Model structures with different cross-linking rates: (a) 0%; (b) 32.81%; (c) 64.06%; (d) 90.00%.

DownLoad: Full-Size Img PowerPoint

图 4 环氧树脂热导率与交联率的函数关系

Figure 4. Functional relationship between thermal conductivity and cross-linking rate of epoxy resin.

DownLoad: Full-Size Img PowerPoint

图 5 不同粒径复合物　(a) 结构图; (b) 热导率; (c) 径向分布函数

Figure 5. Different particle size composites: (a) Structure diagram; (b) thermal conductivity; (c) radial distribution function.

DownLoad: Full-Size Img PowerPoint

图 6 不同粒径复合物的自由体积示意图　(a) 1.0 nm; (b) 1.2 nm; (c) 1.6 nm; (d) 2.0 nm

Figure 6. Free volume diagram of composites with different particle sizes: (a) 1.0 nm; (b) 1.2 nm; (c) 1.6 nm; (d) 2.0 nm.

DownLoad: Full-Size Img PowerPoint

图 7 不同颗粒数复合物　(a) 结构图; (b) 热导率; (c) 振动态密度图谱

Figure 7. Composites with different particle numbers: (a) Structure diagram; (b) thermal conductivity; (c) vibrational density of state.

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图 8 不同质量分数复合物的热导率

Figure 8. Thermal conductivity of composites with different mass fractions.

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表 1 不同粒径复合物的自由体积

Table 1. Free volumes of composites with different particle sizes.

金刚石粒径/nm	金刚石质量分数/%	占有体积/Å³	自由体积/Å³	自由体积分数/%
0	0	31583.63	7827.48	19.86
1.0	4.18	32166.77	6164.56	16.08
1.2	7.84	32714.45	5616.88	14.65
1.4	11.92	33333.22	4998.11	13.04
1.6	15.69	33869.13	4462.21	11.64
1.8	20.91	34920.74	3410.59	8.90
2.0	26.15	35555.49	2775.84	7.24

DownLoad: CSV

表 2 不同颗粒数复合物的自由体积

Table 2. Free volumes of composites with different particle numbers.

金刚石数目/个	金刚石质量分数/%	占有体积/Å³	自由体积/Å³	自由体积分数/%
0	0	31583.63	7827.48	19.86
1	4.18	32166.77	6164.56	16.08
2	8.03	32852.43	5478.91	14.29
3	11.58	33638.61	4692.72	12.24
4	14.86	33818.23	4513.11	11.77
6	20.75	35202.99	3128.34	8.16
10	30.38	36910.39	1420.94	3.71

DownLoad: CSV

[1]	Singha S, Thomas M J 2008 IEEE Trans. Dielectr. Electr. Insul. 15 2 Google Scholar
[2]	Li M, Zhou H, Zhang Y, Liao Y, Zhou H 2018 Carbon 130 295 Google Scholar
[3]	Han Y, Shi X, Wang S, Ruan K, Lu C, Guo Y, Gu J 2021 Composites Part B 210 108666 Google Scholar
[4]	Chen H, Ginzburg V V, Yang J, Yang Y, Liu W, Huang Y, Du L, Chen B 2016 Prog. Polym. Sci. 59 41 Google Scholar
[5]	Liu X, Yu X, Yang Z, Zhuang X, Guo H, Luo X, Chen J, Liang Y, Chen Y 2023 J. Electron. Mater. 52 2831 Google Scholar
[6]	Wang X, Sun L, Zhang X, Zhang S, Wang J, Zhang Y 2020 J. Mol. Liq. 309 113162 Google Scholar
[7]	Wang Y, Chang Z, Gao K, Li Z, Hou G, Liu J, Zhang L 2021 Polymer 224 123697 Google Scholar
[8]	Lian G, Tuan C C, Li L, Jiao S, Wang Q, Moon K S, Cui D, Wong C P 2016 Chem. Mater. 28 6096 Google Scholar
[9]	Wu H, Gao J, Xiong Y, Zhu Q, Yue Y 2021 Int. J. Heat Mass Transfer 178 121634 Google Scholar
[10]	Nejad S M, Srivastava R, Bellussi F M, Thielemann H C, Asinari P, Fasano M 2021 Int. J. Therm. Sci. 159 106588 Google Scholar
[11]	Fasanella N A, Sundararaghavan V 2016 JOM 68 1396 Google Scholar
[12]	Yang K, Chen W, Zhao Y, Ding L, Du B, Zhang S, Yang W 2021 Compos. Sci. Technol. 221 109178 Google Scholar
[13]	Kang E, Choi S, Choi C, Shim S E 2012 Colloids Surf. A 415 255 Google Scholar
[14]	Cho H B, Konno A, Fujihara T, Suzuki T, Tanaka S, Jiang W, Suematsu H, Niihara K, Nakayama T 2011 Compos. Sci. Technol. 72 112 Google Scholar
[15]	Sun M, Yang L, Liu K, Gao G, Su Z, Gao G, Liu B, Wang W, Han J, Dai B 2019 Composites Part A 127 105618 Google Scholar
[16]	Neitzel I, Mochalin V, Knoke I, Palmese G R, Gogotsi Y 2011 Compos. Sci. Technol. 71 710 Google Scholar
[17]	Alder B J, Wainwright T E 1957 J. Chem. Phys. 27 1208 Google Scholar
[18]	Yang X, Wang X, Wang W, Fu Y, Xie Q 2020 Int. J. Heat Mass Transfer 159 120105 Google Scholar
[19]	Zhu M, Li J, Chen J, Song H, Zhang H 2019 Comput. Mater. Sci. 164 108 Google Scholar
[20]	Li C, Strachan A 2011 Polymer 52 2920 Google Scholar
[21]	Hansen J P, McDonald I R 2013 Theory of Simple Liquids: with Applications to Soft Matter (4th Ed.) (Washington, DC: Academic Press) pp311–362
[22]	Alaghemandi M, Müller-Plathe F, Böhm M C 2011 J. Chem. Phys. 135 184905 Google Scholar
[23]	Shavikloo M, Kimiagar S 2017 Comput. Mater. Sci. 139 330 Google Scholar
[24]	Müller-Plathe F 1997 J. Chem. Phys. 106 6082 Google Scholar
[25]	Ikeshoji T, Hafskjold B 1994 Mol. Phys. 81 251 Google Scholar
[26]	Choi J, Shin H, Cho M 2016 Polymer 89 159 Google Scholar
[27]	Xiong Q L, Meguid S A 2015 Eur. Polym. J. 69 1 Google Scholar
[28]	Li S, Yu X, Bao H, Yang N 2018 J. Phys. Chem. C 122 13140 Google Scholar
[29]	Huo R, Zhang Z, Athir N, Fan Y, Liu J, Shi L 2020 Phys. Chem. Chem. Phys. 22 19735 Google Scholar
[30]	Wan X, Demir B, An M, Walsh T R, Yang N 2021 Int. J. Heat Mass Transfer 180 121821 Google Scholar
[31]	Liu X, Rao Z 2020 Comput. Mater. Sci. 172 109298 Google Scholar
[32]	徐文雪, 梁新刚, 徐向华, 祝渊 2020 物理学报 69 196601 Google Scholar Xu W X, Liang X G, Xu X H, Zhu Y 2020 Acta Phys. Sin. 69 196601 Google Scholar
[33]	An M, Demir B, Wan X, Meng H, Yang N, Walsh T R 2019 Adv. Theor. Simul. 2 1800153 Google Scholar
[34]	Kikugawa G, Desai T G, Keblinski P, Ohara T 2013 J. Appl. Phys. 114 034302 Google Scholar
[35]	Pashayi K, Fard H R, Lai F, Iruvanti S, Plawsky J, Borca-Tasciuc T 2012 J. Appl. Phys. 111 104310 Google Scholar
[36]	Fu J, Shi L, Zhang D, Zhong Q, Chen Y 2010 Polym. Eng. Sci. 50 1809 Google Scholar
[37]	Swartz E T, Pohl R O 1989 Rev. Mod. Phys. 61 605 Google Scholar
[38]	Wang Y, Yang C, Mai Y W, Zhang Y 2016 Carbon 102 311 Google Scholar
[39]	Wang Y, Yang C, Pei Q X, Zhang Y 2016 ACS Appl. Mater. Interfaces 8 8272 Google Scholar
[40]	Li C, Medvedev G A, Lee E W, Kim J, Caruthers J M, Strachan A 2012 Polymer 53 4222 Google Scholar

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