[1]闫利文,翁凌,李红霞,等.聚酰胺酸盐法制备纳米SiO2/PI复合薄膜[J].深圳大学学报理工版,2014,31(1):77-82.[doi:10.3724/SP.J.1249.2014.01077]
　Yan Liwen,Weng Ling,Li Hongxia,et al.Nano-SiO2/PI composite films prepared via poly(amic acid) salts process[J].Journal of Shenzhen University Science and Engineering,2014,31(1):77-82.[doi:10.3724/SP.J.1249.2014.01077]
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聚酰胺酸盐法制备纳米SiO2/PI复合薄膜()
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《深圳大学学报理工版》[ISSN:1000-2618/CN:44-1401/N]

卷:
第31卷
期数:
2014年第1期
页码:
77-82
栏目:
材料科学
出版日期:
2014-01-14

文章信息/Info

Title:
Nano-SiO2/PI composite films prepared via poly(amic acid) salts process
文章编号:
20140111
作者:
闫利文1; 翁凌1; 李红霞1; 夏乾善1; 崔巍巍1; 刘立柱1;  2
1）哈尔滨理工大学材料科学与工程学院，哈尔滨 150040
2）哈尔滨理工大学工程电介质及其应用教育部重点实验室，哈尔滨 150080
Author(s):
Yan Liwen1;  Weng Ling1;  Li Hongxia1;  Xia Qianshan1;  Cui Weiwei1;  and Liu Lizhu1;  2
1）School of Materials Science and Engineering, Harbin University of Science and Technology, Harbin 150040, P.R.China
2）Key Laboratory of Engineering Dielectrics and Its Application, Ministry of Education, Harbin University of Science and Technology, Harbin 150080, P.R.China
关键词:
复合薄膜; 聚酰氨酸盐; 氧化硅; 聚酰亚胺; 纳米分散; 热分解; 电击穿场强; 绝缘性
Keywords:
composite film;  poly (amic acid) salts;  silica;  polyimide;  nanoscale dispersion;  thermal decomposition;  breakdown field strength;  insulativity
分类号:
TM 215.3
DOI:
10.3724/SP.J.1249.2014.01077
文献标志码:
A
摘要:
以均苯四甲酸二酐和4, 4′-二胺基二苯醚为聚合单体，制备聚酰胺酸，利用有机碱三乙胺与聚酰胺酸中—COOH的中和反应，制备具有水溶性的聚酰亚胺前驱体——聚酰胺酸盐；将正硅酸乙酯的水溶液加入聚酰胺中，利用正硅酸乙酯的水解使得水解产物SiO2以纳米尺寸均匀分散在聚酰胺中，经热亚胺化处理制备出SiO2质量分数不同的SiO2/PI复合薄膜．采用扫描电子显微镜对复合薄膜的断面微观结构进行分析，实验结果表明，SiO2在PI基体内分散均匀．当SiO2质量分数为20%时，仍未出现团聚现象．复合薄膜的力学性能、热性能及电性能测试结果显示，由于SiO2的生成，复合薄膜的力学性能稍有下降；薄膜的热分解温度随着SiO2质量分数的增大逐渐升高；复合薄膜的电击穿场强由纯PI薄膜的160.0 kV/mm提高到229.8 kV/mm（SiO2质量分数16%），随着SiO2质量分数的增大，复合薄膜的体积电阻率和表面电阻率均呈先增后减趋势；引入SiO2显著提高了复合薄膜的绝缘性，拓展了其在电气绝缘领域的应用．
Abstract:
A water-soluble polyimide precursor called polyamide acid salt (PAAs) was synthesized via the neutralization reaction of triethylamine (TEA) and polyamide acid (PAA). PAA was generated from the monomer pyromellitic dianhydride (PMDA) and 4,4′-oxydianline (ODA) beforehand. A series of silica/polyimide (SiO2/PI) composite films with different silica mass fraction were prepared from tetraethyl orthosilicate (TEOS) and PAAs. The uniform dispersion of SiO2 in PI matrix benefited from the direct hydrolysis of TEOS in PAAs. The microscopic morphology of composite films was characterized by scanning electron microscope (SEM). The dispersion of SiO2 in PI matrix was homogeneous even though the SiO2 mass fraction reaches 20%, which shows the excellent compatibility between SiO2 and PI in the composite films prepared by Poly (amic acid) salts. The mechanical, thermal performance and electrical properties of the SiO2/PI composite films were studied. The results show that both the tensile strength and the elongation at break decrease slightly with increasing SiO2 mass fraction. The thermal decomposition temperature of the composite films increases gradually with the increase of the mass fraction of SiO2. The breakdown field strength of the SiO2/PI composite film, 16% mass fraction of SiO2 addition, is 229.8 kV/mm while the pure PI film is 160.0 kV/mm. The volume resistivity of the composite films, as well as the surface resistivity, increases firstly and then decreases synchronously with the increase of the mass fraction of SiO2. The insulativity of the composite films is significantly improved by the introduction of SiO2, which facilitates the application of the PI composite films in the field of electrical insulation.

参考文献/References:

［1］ Srivastava R, Banerjee S, Jehnichen D, et al. In situ preparationofpolyimidecompositesbasedonfunctionalized carbon nanotubes［J］. Macromolecular Materials and Engineering, 2009, 294(2): 96-102.
［2］ Shen Jie, Li Xiaolong, Zhang Ying, et al. Synthesis and characterization of highly soluble and optically transparent polyimides derived from novel fluorinated pyridine-containing aromatic diamine［J］. High Performance Polymers, 2013, 25(3): 268-277.
［3］ Zheng Zhuoyong, Yu Guanglong, Zhang Zhijian, et al. Characterization of SiO2/polyimide/SiO2 composite films and its applications in field emission display［J］. Journal of Vacuum Science and Technology, 2012, 32(3): 214-218.(in Chinese)
郑灼勇，于光龙，张志坚，等. SiO2/聚酰亚胺/SiO2复合薄膜绝缘性能及基于聚酰亚胺复合薄膜的后栅型场致发射性能的研究［J］. 真空科学与技术学报，2012，32(3): 214-218.
［4］ Weng Ling, Liu Lizhu, Yang Liqian, et al. Preparation, morphology and properties of nano-silica-alumina co-doped polyimide three-layer composite films［J］. Polymers and Polymer Composites, 2011, 19(2):189-195.
［5］ Min Chunkuo，Wu Taibor，Yang Weita，et al．Functionalized mesoporous silica/polyimide nanocomposite thin films with improved mechanical properties and low dielectric constant［J］. Composites Science and Technology, 2008, 68(6): 1570-1578.
［6］ Akhter T, Saeed S, Siddiqi H, et al. Preparation and characterization of novel polyimide-silica hybrids［J］. Polymers for Advanced Technologies, 2013, 24(4): 407-414.
［7］ Huang Jieyang, Zhang Peng, Wang Xu, et al. Crystallization of inorganic silica based on interaction between polyimide and silica by sol-gel method［J］. Journal of Sol-Gel Science and Technology, 2013, 66(2): 193-198.
［8］ Chen Xingui, Guo Jingdong, Zheng Bing, et al. Investigation of thermal expansion of PI/SiO2 composite films by CCD imaging technique from -120 to 200 ℃［J］. Composites Science and Technology, 2007, 67(14): 3006-3013.
［9］ Guo Jiao, Nguyen Baochau N, Li Lichun, et al. Clay reinforced polyimide/silica hybrid aerogel［J］. Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2013, 24(1): 7211-7221.
［10］ Fan Yong, Li Yanru, Chen Hao. Research progress on corona resistant property and breakdown strength of inorganic nano hybrid PI films［J］. Journal of Harbin University of Science and Technology, 2012, 17(1): 1-5.(in Chinese)
范勇, 李彦如, 陈昊. 纳米杂化聚酰亚胺薄膜耐电晕性和击穿场强研究进展［J］. 哈尔滨理工大学学报, 2012, 17(1): 1-5.
［11］ Yang Yang, Jia Zhenxing, Wang Ying, et al. Preparation of hemispherical polyimide particles by inverse emulsion technique from poly(amic acid) ammonium salts［J］. Colloid and Polymer Science, 2013, 291(5): 1049-1055.
［12］ Wu Wei, Wang Kai, Zhan Maosheng. Preparation and performance of polyimide-reinforced clay aerogel composites［J］. Industrial and Engineering Chemistry Research, 2012, 51(39): 12821-12826.
［13］ Huang Shuhui, Don Trongming, Lai Weichi, et al. Porous structure and thermal stability of photosensitive silica/polyimide composites prepared by sol-gel process［J］. Journal of Applied Polymer Science, 2009, 114(4): 2019-2029.
［14］ Cai Dongdan, Su Jianfeng, Huang Mei, et al. Synthesis, characterization and hydrolytic stability of poly (amic acid) ammonium salt［J］. Polymer Degradation and Stability, 2011, 96(12): 2174-2180.
［15］ Ha Youri, Choi Myeoncheon, Jo Namju, et al. Polyimide multilayer thin films prepared via spin coating from poly(amic acid) and poly(amic acid) ammonium salt［J］. Macromolecular Research, 2008, 16(8): 725-733.
［16］ Lee T，Park S，Jung Y，et al．Preparation and characterization of polyimide/mesoporous silica hybrid nanocomposites based on water-soluble poly(amic acid) ammonium salt［J］. European Polymer Journal, 2009, 45(1): 19-29.

备注/Memo

备注/Memo:
Received：2013-10-09；Accepted：2013-12-15
Foundation：National Natural Science Foundation of China(51177030); Natural Science Foundation of Heilongjiang Province(E201224)
Corresponding author：Associate professor Weng Ling. E-mail: wengling79@163.com
Citation：Yan Liwen, Weng Ling, Li Hongxia,et al. Nano-SiO2/PI composite films prepared via poly(amic acid) salts process［J］. Journal of Shenzhen University Science and Engineering, 2014, 31(1): 77-82.（in Chinese）
基金项目：国家自然科学基金资助项目（51177030）；黑龙江省自然科学基金资助项目（E201224）
作者简介：闫利文（1989-），男（汉族），内蒙古自治区乌兰察布市人，哈尔滨理工大学硕士研究生. E-mail: levenman@126.com
引文：闫利文，翁凌，李红霞，等.聚酰胺酸盐法制备纳米SiO2/PI复合薄膜［J］. 深圳大学学报理工版，2014，31（1）：77-82.
更新日期/Last Update: 2014-01-08