文献类型：期刊文献

中文题名：基于材料基因组方法的含硅芳炔树脂的设计与合成

英文题名：Accelerating the Design and Synthesis of Heat-resistant Silicon-containing Arylacetylene Resins by a Material Genome Approach

作者：楚明[1];朱峻立[1];王立权[1];林嘉平[1];杜磊[1];蔡春华[1]

机构：[1]华东理工大学材料科学与工程学院上海市先进聚合物重点实验室

年份：2019

卷号：50

期号：11

起止页码：1219

中文期刊名：高分子学报

外文期刊名：Acta Polymerica Sinica

收录：CSTPCD;;Scopus;WOS:【SCI-EXPANDED(收录号:WOS:000497774600009)】；北大核心:【北大核心2017】；CSCD:【CSCD2019_2020】；

基金：国家自然科学基金(基金号51833003)资助项目

语种：中文

中文关键词：材料基因组;含硅芳炔;固化温度;耐热性能

外文关键词：Material genome approach;Silicon-containing arylacetylene;Curing temperature;Heat resistance

摘要：建立了一种针对耐高温树脂设计的材料基因组方法,运用该方法设计筛选了一种固化温度低(加工性能优良)、耐热性能优异的新型含硅芳炔树脂-聚(二苯基硅烷-乙炔基-萘-乙炔基)树脂(简称PSNP树脂).基于理论设计的结果,通过Sonogashira偶联法制得了2,7-二乙炔基萘,然后以二氯二苯基硅烷和2,7-二乙炔基萘为反应物合成了PSNP树脂.通过傅里叶变换红外光谱(FTIR)、核磁共振氢谱(~1H-NMR)等方法对PSNP树脂的结构进行了表征.利用示差扫描量热分析(DSC)研究了PSNP树脂的固化过程,结果表明PSNP树脂的固化放热峰的峰值温度和固化放热焓均低于传统的含硅芳炔树脂(PSA树脂),改善了树脂的加工性能.热失重分析(TGA)表明,固化后的PSNP树脂具有优异的耐热性.树脂的性能与理论设计的结果相符,证实了材料基因组方法对于新型含硅芳炔树脂的设计筛选的有效性.
We developped a material genome approach to accelerate the design and synthesis of novel heatresistant silicon-containing arylacetylene resins. The material genome approach is based on the consideration that silicon-containing arylacetylene resins can be regard as a combination of silane and diyne units which can be defined as genes used for combination screening. The approach presented here contains two steps. In the first step,various kinds of diynes were collected from the chemical database as candidate structures;the bond dissociation energy(BDE) reflecting heat resistance of resins was calculated;the candidate structures were preliminarily screened with the criteria of BDE;and finally 16 diynes with high BDE were obtained. In the second step, LUMO-HOMO and 50% decomposition temperature(Td50) were calculated by density functional theory and molecular connection index method, respectively;and the optimized gene was obtained out of 16 candidate structures. The screened resin is poly(diphenylsilylene-ethynylene-naphthalene-ethynylene)(abbreviated as PSNP) containing the gene of 2,7-diethynylnaphthalene. To verify the screened results, we first synthsized the PSNP by Sonogashira coupling of dichlorodiphenylsilane and 2,7-diethynylnaphthalene. The molecular structure of PSNP resin was characterized by Fourier transform infrared spectroscopy(FTIR) and nuclear magnetic resonance(1 H-NMR). The curing process of PSNP resin was studied by differential scanning calorimetry(DSC). The results show that the curing peak temperature(Tpeak) of PSNP and the enthalpy of exothermic reaction are 212 ℃ and 173.8 J/g,respectively, which are lower than those of traditional poly(silylene-acetylenearyleneacetylene) resin(PSA). The cured PSNP resin exhibits excellent heat-resistance, where the 5% decomposition temperature(Td5) of the cured PSNP resin is 561 ℃. The properties of the resin are consistent with the theoretical design results, which confirms the validity of material genome method for structural screening of new silicon-containing arylacetylene resins.