CNTs阵列增强石蜡/硅橡胶复合相变垫片的散热性能研究

doi:10.11949/0438-1157.20220297

化工学报 ›› 2022, Vol. 73 ›› Issue (7): 2874-2884.DOI: 10.11949/0438-1157.20220297

CNTs阵列增强石蜡/硅橡胶复合相变垫片的散热性能研究

蔡楚玥¹(),方晓明^1,²,张正国^1,^2,³(),凌子夜^1,²

^1.华南理工大学传热强化与过程节能教育部重点实验室，广东广州 510640
^2.广东省热能高效储存与利用工程技术研究中心，广东广州 510640
^3.华南理工大学珠海现代产业创新研究院，广东珠海 519175

收稿日期:2022-03-02 修回日期:2022-04-24 出版日期:2022-07-05 发布日期:2022-08-01
通讯作者: 张正国
作者简介:蔡楚玥（1997—），女，硕士研究生，374591187@qq.com
基金资助:
国家重点研发计划项目(2020YFA0210704)

Enhancing heat dissipation performance of paraffin/silicone rubber phase change thermal pad by introducing carbon nanotubes

Chuyue CAI¹(),Xiaoming FANG^1,²,Zhengguo ZHANG^1,^2,³(),Ziye LING^1,²

^1.Key Laboratory of Enhanced Heat Transfer and Energy Conservation, Ministry of Education, South China University of Technology, Guangzhou 510640, Guangdong, China
^2.Guangdong Engineering Technology Research Center of Efficient Heat Storage and Application, South China University of Technology, Guangzhou 510640, Guangdong, China
^3.South China University of Technology-Zhuhai Institute of Modern Industrial Innovation, Zhuhai 519175, Guangdong, China

Received:2022-03-02 Revised:2022-04-24 Online:2022-07-05 Published:2022-08-01
Contact: Zhengguo ZHANG

摘要/Abstract

摘要：

电子技术的高速发展对散热技术提出了更高的要求，热界面材料作为散热技术的关键材料之一，面临着提高热导率以及减小传热热阻的挑战。将垂直碳纳米管阵列(VACNTs)和固-液相变材料石蜡(PA)与硅橡胶(SR)复合，研制了一种新型VACNTs/PA/SR复合相变垫片。研究表明，通过磁场校准方法可以使表面改性的镀镍多壁CNTs在SR中实现垂直定向排列，所得VACNTs/SR垫片较CNTs随机排列的垫片具有更高的热导率，并确定VACNTs/SR垫片中CNTs的适宜含量为6%(质量)，对应垫片的热导率可达0.71 W/(m·K)。对于固定CNTs含量为6%(质量)但PA含量不同的一系列VACNTs/PA/SR相变垫片，PA的添加量不大于12.5%(质量)时，相变垫片克服了液态PA的泄漏问题；相变垫片在PA发生固-液相变后表现出硬度显著下降，热阻减少可达55.14%，并具备优异的热可靠性。将最佳VACNTs/SR垫片样品及最佳VACNTs/PA/SR相变垫片样品进行散热性能对比发现，与使用VACNTs/SR垫片的情况相比，使用VACNTs/PA/SR相变垫片时的模拟芯片不仅在温度上升阶段的升温速率更小，而且当芯片温度达到平衡后对应的平衡温度也更低，降低了3.5℃，显示出更好的散热性能。VACNTs/PA/SR相变垫片优良的特性和散热性能使其在电子设备散热领域具有良好的应用前景。

关键词: 碳纳米管, 相变, 热阻, 热界面材料, 传热, 电子材料

Abstract:

The rapid development of electronic technology has put forward higher requirements for heat dissipation technology. As one of the key materials of heat dissipation technology, thermal interface materials are facing the challenge of improving thermal conductivity and reducing heat transfer resistance. In this paper, a novel VACNTs/PA/SR phase change gasket was developed by combining vertically aligned carbon nanotubes (VACNTs) and a solid-liquid phase change material, paraffin (PA), with silicone rubber (SR). It is shown that the magnetic field calibration method could make the surface modified nickel coated multi-wall CNTs vertically oriented in SR, and the obtained VACNTs/SR gaskets had higher thermal conductivity than the gaskets with CNTs randomly arranged. The appropriate content of CNTs in the VACNTs/SR gasket was determined to be 6% (mass), and the corresponding gasket reached a thermal conductivity of 0.71 W /(m·K). As for a series of VACNTs/PA/SR phase change gaskets at different loadings of PA, it is found that, the leakage problem of the liquid PA was overcome at the addition of PA of less than 12.5% (mass). After the solid-liquid phase transition of PA, the gasket shows a significant decrease in hardness, and even the thermal resistance can be reduced by up to 55.14%, and has excellent thermal reliability. By comparing the heat dissipation performance between the optimal VACNTs/SR gasket and the optimal VACNTs/PA/SR phase change gasket it is revealed that, when employing the phase change gasket, the simulation chip not only showed a lower rising rate in temperature but also had a lower equilibrium temperature with a decline of 3.5℃, suggesting the better heat dissipation performance of the VACNTs/PA/SR phase change gasket than the VACNTs/SR gasket. The VACNTs/PA/SR phase change gasket shows promise in the fields of electronic equipment heat dissipation.

Key words: carbon nanotubes, phase change, thermal resistance, thermal interface materials, heat transfer, electronic materials

中图分类号:

TB 34

蔡楚玥, 方晓明, 张正国, 凌子夜. CNTs阵列增强石蜡/硅橡胶复合相变垫片的散热性能研究[J]. 化工学报, 2022, 73(7): 2874-2884.

Chuyue CAI, Xiaoming FANG, Zhengguo ZHANG, Ziye LING. Enhancing heat dissipation performance of paraffin/silicone rubber phase change thermal pad by introducing carbon nanotubes[J]. CIESC Journal, 2022, 73(7): 2874-2884.

图/表 15

图1 VACNTs/PA/SR相变垫片的制备流程示意图

Fig.1 Schematic diagram for preparing VACNTs/PA/SR phase change thermal pads

图2 评估垫片散热性能的实验装置1—热电偶;2—陶瓷加热片;3—隔热底座;4—风扇;5—热管换热器;6—螺钉

Fig.2 Experimental set-up for evaluating heat dissipation performance of thermal pads

图3 CNTs（a）、氧化CNTs（b）和表面改性CNTs（c）的红外光谱

Fig.3 FT-IR spectra of CNTs（a）, acid treated CNTs（b） and surface modified CNTs（c）

图4 不同静置时间下样品在硅油中的分散情况照片A—CNTs; B—氧化CNTs; C—表面改性CNTs

Fig.4 Photographs of different CNTs dispersions at different storing durationsA—CNTs; B—acid treated CNTs; C—surface modified CNTs

图5 垫片的横截面SEM图像

Fig.5 Cross-section SEM images of thermal pads

图6 CNTs质量分数不同的CNTs/SR和VACNTs/SR垫片热导率

Fig.6 Thermal conductivity of the CNTs/SR和VACNTs/SR thermal pads containing different mass fractions of CNTs

图7 硅橡胶、表面改性CNTs和TIM-6的红外光谱

Fig.7 FT-IR spectra of silicone elastomer, surface modified CNTs and TIM-6

图8 含有不同PA质量分数的VACNTs/PA/SR相变垫片的DSC曲线

Fig.8 DSC curves of the VACNTs/PA/SR phase change thermal pads containing different mass fractions of PA

表1 含有不同质量分数PA相变垫片的相变特性

Table 1 Phase change characteristics of phase change thermal pads containing different mass fractions of PA

样品	w/%	T_m/℃	H_m/(J/g)	T_f/℃	H_f/(J/g)	η/%
PA	100	49.0	199.1	52.4	198.7	100
PCTIM-1	5.0	51.8	8.5	53.0	7.8	4.1
PCTIM-2	7.5	51.0	12.9	52.2	12.1	6.3
PCTIM-3	10.0	51.0	17.7	52.6	17.1	8.8
PCTIM-4	12.5	50.5	23.7	53.2	23.2	11.8
PCTIM-5	15.0	50.1	26.6	52.8	25.8	13.2

图9 不同PA质量分数的VACNTs/PA/SR相变垫片在加热过程中的质量损失率

Fig.9 Mass loss percentages of the phase change thermal pads containing different mass fractions of PA during the heating

图10 含有不同PA质量分数的VACNTs/PA/SR相变垫片的热导率、硬度及热阻

Fig.10 Thermal conductivity, hardness, and resistance of the thermal pads containing different mass fractions of PA under different temperature

图11 PCTIM-4及其组分的红外光谱以及循环100次前后的DSC曲线

Fig.11 FT-IR spectra of PCTIM-4 and its components, DSC curves of PCTIM-4 before and after 100 cycles

图12 在不同功率下不使用垫片（空载）和使用不同垫片时模拟芯片的温升曲线

Fig.12 Temperature rise curves of the simulative chip when employing no thermal pads and the different thermal pads at different heating power

表2 在不同功率下不使用（空载）和使用不同垫片时模拟芯片的平衡温度

Table 2 Equilibrium temperatures of the simulative chip when employing no TIM and different TIMs at different heating power

功率/W	T_空载/℃	T_TIM/℃	T_PCTIM/℃	ΔT/℃
100	141.0	130.6	129.5	1.1
30	109.1	98.2	96.5	1.7
20	81.4	71.9	69.8	2.1
10	57.0	48.7	45.2	3.5

表3 TIM-6和PCTIM-4的特性参数

Table 3 Characteristics of TIM-6 and PCTIM-4

性能参数	TIM-6	PCTIM-4
热导率/(W/(m·K))	0.71	0.71
厚度/mm	0.98	0.98
硬度/HA	47.5	34.7
热阻/(K·cm²/W)	19.1483	15.2650

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CNTs阵列增强石蜡/硅橡胶复合相变垫片的散热性能研究

Enhancing heat dissipation performance of paraffin/silicone rubber phase change thermal pad by introducing carbon nanotubes

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