具有rGO三维导热网络结构聚酰亚胺复合薄膜的制备及性能

魏世洋; 郑智博; 余桥溪; 范振国; 刘四委; 池振国; 张艺; 许家瑞

doi:10.11777/j.issn1000-3304.2018.18253

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具有rGO三维导热网络结构聚酰亚胺复合薄膜的制备及性能

研究论文 | 更新时间：2021-01-26

- 具有rGO三维导热网络结构聚酰亚胺复合薄膜的制备及性能
- Enhanced Thermal Conductivity of PI Films by Strengthening Three-dimensional rGO Network Template
- 高分子学报 2019年50卷第4期页码：402-409
- 作者机构：
  
  中山大学聚合物复合材料及功能材料教育部重点实验室高性能树脂基复合材料广东省重点实验室广东省高性能有机聚合物光电功能薄膜工程技术研究中心化学学院　广州 510275
- 作者简介：
  
  E-mail: ceszy@mail.sysu.edu.cn Yi Zhang, E-mail: ceszy@mail.sysu.edu.cn
  E-mail: xjr@mail.sysu.edu.cn Jia-rui Xu, E-mail: xjr@mail.sysu.edu.cn
- 基金信息：
  
  国家重点基础研究发展计划(973计划，项目号 2014CB643605)、国家自然科学基金(基金号 51873239)、广东省“特支计划”科技创新领军人才项目(项目号 2016TX03C295)、广东省前沿与关键技术创新专项(项目号 2015B090915003, 2015B090913003)、中国博士后科学基金(基金号 2017M612801)和高等学校基本科研业务费(项目号161gzd08)资助()
- DOI：10.11777/j.issn1000-3304.2018.18253
  中图分类号：
- 纸质出版日期：2019-4，
  
  网络出版日期：2019-2-25，
  
  收稿日期：2018-11-23，
  
  修回日期：2018-1-2，
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魏世洋, 郑智博, 余桥溪, 范振国, 刘四委, 池振国, 张艺, 许家瑞. 具有rGO三维导热网络结构聚酰亚胺复合薄膜的制备及性能[J]. 高分子学报, 2019,50(4):402-409.

Shi-yang Wei, Zhi-bo Zheng, Qiao-xi Yu, Zhen-guo Fan, Si-wei Liu, Zhen-guo Chi, Yi Zhang, Jia-rui Xu. Enhanced Thermal Conductivity of PI Films by Strengthening Three-dimensional rGO Network Template[J]. Acta Polymerica Sinica, 2019,50(4):402-409.
魏世洋, 郑智博, 余桥溪, 范振国, 刘四委, 池振国, 张艺, 许家瑞. 具有rGO三维导热网络结构聚酰亚胺复合薄膜的制备及性能[J]. 高分子学报, 2019,50(4):402-409. DOI： 10.11777/j.issn1000-3304.2018.18253.

Shi-yang Wei, Zhi-bo Zheng, Qiao-xi Yu, Zhen-guo Fan, Si-wei Liu, Zhen-guo Chi, Yi Zhang, Jia-rui Xu. Enhanced Thermal Conductivity of PI Films by Strengthening Three-dimensional rGO Network Template[J]. Acta Polymerica Sinica, 2019,50(4):402-409. DOI： 10.11777/j.issn1000-3304.2018.18253.

摘要

为了使还原氧化石墨烯(rGO)的面内导热方向与复合物材料散热方向一致，提高rGO在复合材料中的导热效率，更大程度地释放rGO的导热潜力，采用冷冻干燥的方法处理rGO的聚酰胺酸(PAA)分散液，得到PAA黏结的rGO三维网络结构，热酰亚胺化之后得到聚酰亚胺(PI)加固的rGO三维网络结构模板(3DrGO-PI). 使用10 wt%的PAA胶液浇铸上述3DrGO-PI模板，制备得到含有rGO三维导热网络结构的3DrGO/PI复合薄膜. 结果表明，所得到的复合薄膜具有良好的导热性能，当rGO的含量为8 wt%时，3DrGO/PI复合薄膜导热系数达到1.57 W·m

−1

·K

−1

，为纯PI导热系数的8.72倍. 同时复合薄膜具有较好的热稳定性，随着rGO含量的增加，薄膜的

上升，热膨胀系数(CTE)下降，热性能更稳定.

Abstract

In this work

high thermal conductive polyimide (PI) composites with reduced graphene oxide (rGO) as filler were prepared. In order to improve the thermal conductivity of rGO in the PI composites

rGO should form heat conductive paths in PI matrix

and the in-plane direction of rGO should be consistent with the heat dissipation direction of composite materials. Therefore

three-dimensional rGO networks (3DrGO) were prepared by freeze-drying technology to construct an effective thermal conductive path in PI matrix. In order to stabilize 3DrGO networks during the preparation process of PI composites

the 3DrGO networks were adhered and reinforced by PI. The process includes: (1) the rGO dispersion containing 3 wt% polyamide acid (PAA) was freeze-dried to prepare the PAA-reinforced 3DrGO network (3DrGO-PAA); (2) the 3DrGO-PAA was treated by thermal imidization to obtain the PI-reinforced 3DrGO network (3DrGO-PI); (3) 10 wt% PAA was cast onto the 3DrGO-PI template and imidized at 100

200

and 350 °C for 1 h

respectively

at each temperature to obtain the 3DrGO-PI/PI composite films. The 3DrGO-PI/PI composite film exhibits the thermal conductivity of 1.57 W·m

−1

·K

−1

with 8 wt% rGO (772% enhancement compared to that of neat PI film). Whereas the PI composite films with random distributed rGO (rGO/PI composite film) or unreinforced 3DrGO (3DrGO-water/PI composite film) only exhibit the thermal conductivity of 0.51 W·m

−1

·K

−1

(183% enhancement compared to that of neat PI film) or 1.02 W·m

−1

·K

−1

(467% enhancement compared to that of neat PI film)

respectively. All the composite films maintain very good thermal stabilities. The

d5%

(thermal decomposition temperature at 5 wt% weight loss) values of the composite films are higher than that at 540 °C. Compared with that of neat PI

the

s of the composite films are slightly enhanced and relatively higher (higher than 390 °C). The coefficient of thermal expansion (CTE) of the composite films can be greatly decreased by the addition of 3DrGO. The CTE of 3DrGO-PI/PI composite film is as low as 2.16 × 10

–5

/°C when loading 8 wt% 3DrGO.

关键词

聚酰亚胺高导热还原氧化石墨烯三维结构浇铸法

Keywords

PolyimideHigh thermal conductivityReduced graphene oxide3D structureCasting

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