超声强制浸润法制备碳纳米纸/聚合物导热复合材料

任兴国; 孙靖尧; 赵中里; 黄尧; 刘颖; 吴大鸣

doi:10.13801/j.cnki.fhclxb.20200214.001

超声强制浸润法制备碳纳米纸/聚合物导热复合材料

doi: 10.13801/j.cnki.fhclxb.20200214.001

任兴国¹,
孙靖尧^1, ,,
赵中里¹,
黄尧¹,
刘颖²,
吴大鸣^{1, 2}

1.
北京化工大学　机电工程学院，北京 100029
2.
有机-无机复合材料国家重点实验室，北京 100029

基金项目: 国家自然科学基金(51673020)；北京市自然科学基金(2204090)

详细信息

通讯作者:
孙靖尧，博士，副教授，研究方向为聚合物先进制造　E-mail：sunjingyao@mail.buct.edu.cn

中图分类号: TB332
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- 被引次数: 0
出版历程
- 收稿日期: 2019-10-10
- 录用日期: 2020-01-14
- 网络出版日期: 2020-02-14
- 刊出日期: 2020-08-15

Preparation of carbon nanopapers/polymer thermal conductive composite by ultrasonic forced infiltration

1.
College of Mechanical and Electrical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
2.
State Key Laboratory of Organic‐Inorganic Composites, Beijing 100029, China

摘要

摘要: 为实现聚合物基导热复合材料的高效制备，提出了一种利用超声焊接设备实施的超声强制浸润方法。采用真空抽滤方法制备出由碳纳米管(Carbon nanotubes, CNTs)堆叠而成的碳纳米纸(Carbon nanopapers, CNPs), 将CNPs放置在未固化的聚二甲基硅氧烷(Polydimethylsiloxane, PDMS)中，利用超声焊接设备的高频率、高功率超声源进行震荡，凭借超声波的能量传递作用，使液态PDMS逐步浸润到CNPs中。在100℃加热30 min固化后，即得到兼具高柔性和优良导热性能的CNPs/PDMS复合材料。结果表明，相同振幅条件下，CNPs/PDMS复合材料的导热性能随超声处理时长的增加而先上升后下降，并在超声时长为1.9 s时达到最优，热导率达5.781 W/(m·K)。验证了超声强制浸润法高效的制备柔性导热复合材料的可行性。
- 真空抽滤 /
- 超声处理 /
- 强制浸润法 /
- 导热复合材料 /
- 柔性
Abstract: An ultrasonic-assisted forced infiltration method using plastic welding equipment was proposed to realize the efficient preparation of polymer-based thermal conductive composites. The carbon nanopapers (CNPs) consisted by pure carbon nanotubes (CNTs) were prepared using the method of vacuum filtration. The CNPs were placed into uncured polydimethylsiloxane (PDMS) viscous resin. The plastic welding equipment with high frequency and high power ultrasonic source was applied for the ultrasonic treatment, and the liquid PDMS would gradually infiltrated into CNPs depending on the energy transfer effect of ultrasonic wave. The CNPs/PDMS composites with high flexibility and excellent thermal conductivity could be obtained after CNPs/PDMS being cured at 100℃ for 30 min. The experimental results show that under the same amplitude condition, the thermal conductivity of CNPs/PDMS composites would increase first and then decrease with the increase of ultrasonic duration. The thermal conductivity reaches the peak value of 5.781 W/(m·K) when the ultrasonic duration is 1.9 s. The applicability of ultrasonic-assisted forced infiltration method for the preparation of flexible thermal conductive composites is verified in this research work.
- vacuum filtration /
- ultrasonic treatment /
- forced infiltration /
- thermal conductive composites /
- flexibility

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图 1 超声强制浸润方法制备碳纳米纸/聚二甲基硅氧烷(CNPs/PDMS)复合材料的工艺流程图

Figure 1. Process flow chart of preparing carbon nanopapers/polydimethylsiloxane(CNPs/PDMS) composite by ultrasonic forced infiltration method

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图 2 自制红外热成像测试平台

Figure 2. Homemade infrared thermal imaging test platform

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图 3 不同超声处理时间的CNPs/PDMS导热复合材料断面SEM图像

Figure 3. SEM images of CNPs/PDMS thermally conductive composites with different sonication times

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图 4 CNTs/PDMS导热复合材料热导率与超声处理时间关系

Figure 4. Relationship between thermal conductivity of CNTs/PDMS thermal conductive composites and time of ultrasonic treatment

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图 5 不同超声处理时间的CNPs/PDMS导热复合材料的热红外成像

Figure 5. Thermal infrared imaging of CNPs /PDMS thermally conductive composites with different sonication times

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图 6 不同超声处理时间的CNPs/PDMS导热复合材料的温度分布曲线

Figure 6. Temperature distribution curves of CNPs/PDMS thermally conductive composites with different sonication times

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图 7 CNPs/PDMS导热复合材料经0°(a)、90°(b)、180°(c)和360°(d)旋转

Figure 7. CNPs/PDMS thermal conductive composites are rotated by 0°(a), 90°(b), 180°(c) and 360°(d)

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图 8 CNPs/PDMS导热复合材料断裂伸长率与超声处理时间的关系曲线

Figure 8. Relationship between the elongation at break of CNPs/PDMS thermally conductive composites and sonication time

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图 9 不同超声处理时间的CNPs/PDMS导热复合材料的TGA曲线

Figure 9. TGA curves of CNPs/PDMS thermally conductive composites with different sonication times

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表 1 不同超声处理时间的CNPs/PDMS导热复合材料厚度随时间的变化

Table 1. Changes in thickness of CNPs/PDMS thermally conductive composites with different sonication times

Sonication time/s	0	0.5	1.6	1.9	2.2	2.5	2.8
Product thickness/μm	70	90.4	110.3	115.8	110	102.7	95.6

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表 2 不同超声处理时间的CNPs/PDMS导热复合材料的导热性能参数

Table 2. Thermal conductivity parameters of CNPs/PDMS thermally conductive composites with different sonication time

Duration of sonication/s	Specific heat capacity C/ (J(g·K)⁻¹)	Density ρ/ (kg·m⁻³)	Thermal diffusivity α/ (m²·s⁻¹)
1.6	1.326	1.32	2.541
1.9	1.334	1.27	3.412
2.2	1.338	1.25	3.246
2.5	1.324	1.33	3.010
2.8	1.316	1.37	2.879

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表 3 PDMS和CNTs的质量分数

Table 3. Mass fractions of PDMS and CNTs

Parameter	Sonication times/s
Parameter	1.6	1.9	2.2	2.5	2.8
c/wt%	32.1	29.9	27.3	33.7	37.5
PDMS/wt%	73	77	79	72	68
CNTs/wt%	27	23	21	28	32
Note: c—Remaining amount of each time parameter sample at 600℃.

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