Citation: Zhen-guo Fan, Wen-xin Chen, Shi-yang Wei, Teng Liu, Si-wei Liu, Zhen-guo Chi, Yi Zhang, Jia-rui Xu. Quantitative Structure-Property Relationship Study on Dielectric Constant of Polyimide and Its Molecular Structure Design for Low Dielectric Films[J]. Acta Polymerica Sinica, ;2019, 50(2): 179-188. doi: 10.11777/j.issn1000-3304.2018.18183 shu

Quantitative Structure-Property Relationship Study on Dielectric Constant of Polyimide and Its Molecular Structure Design for Low Dielectric Films

Laboratory of Polymeric Composite and Functional Materials, Guangdong Laboratory of High-Performance Polymer Composites, Guangdong Engineering Technology Research Center for High-performance Organic and Polymer Photoelectric Functional Films, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-sen University, Guangzhou 510275

Corresponding author: Yi Zhang, ceszy@mail.sysu.edu.cn Jia-rui Xu, xjr@mail.sysu.edu.cn
Received Date: 15 August 2018
Revised Date: 4 September 2018
Available Online: 18 October 2018

Using the quantum chemical calculation method and the group contribution method, 12 kinds of quantum chemical structure parameters of 61 polyimide molecular structure model units were collected. In order to simplify the calculation process, a segment of the polymer chain was selected and saturated with methyl group, which was used as the model of the polyimide. Through the path analysis, 5 main factors that affect the dielectric constant of the polyimide films were further screened. On this basis, the multiple linear regression (MLR) and artificial neural network (ANN) methods were constructed. Two quantitative structure-property relationship model (QSPR) were built, and the stability and prediction ability of the models were analyzed. The results revealed the intrinsic relationship between the 5 structural parameters and the dielectric constant, i.e., the fluorine content e^−F%, the dipole pitch μ, and the solubility parameter δ of polyimide are positively correlated with the dielectric constant, while the most negative atomic net charge q⁻ and the side length L are negatively correlated with the dielectric constant. MLR-QSPR model has better physical significance and the ANN-QSPR has better accuracy. The accuracy of the models is validated by combining four structures: 6FDA-TriPMPDA, 6FDA-TriPMMDA, 6FDA-TPCF3PDA and 6FDA-TPCF3MDA in our lab. The experimental data show that the average error of the two models is lower than 10% under 1 kHz test condition. Five different fluorine-containing polyimide chain structures were designed according to MLR-QSPR model. The results show that the increase in fluorine content is beneficial to reduce the dielectric constant of the material, but when the fluorine content reaches a certain level, the dielectric constant tends to be stable, which are consistent with the experimental results reported in the literature. When the fluorine content is 34% (k-3), the material possesses the lowest dielectric constant of 2.02. Based on the results of this study, it is believed that QSPR has a good application prospect and theoretical significance in designing new polyimide materials and predicting its properties.
- Polyimide,
- Low dielectric constant,
- Quantitative structure-property relationship,
- Multiple linear regression,
- Artificial neural network
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