Li Xinyu, Han Yue, Qu Jiajun, Chen Qionghai, Wei Yuan, Hou Guanyi, Liu Jun
Key Laboratory of Beijing City on Preparation and Processing of Novel Polymer Materials, Beijing University of Chemical Technology, Beijing 100029, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
Phys Chem Chem Phys. 2023 Mar 29;25(13):9445-9453. doi: 10.1039/d2cp04799c.
Bio-based polyester elastomers have been widely studied by researchers in recent years because of their comprehensive sources of monomers and environmentally friendly characteristics. However, compared with traditional petroleum-based elastomers, the thermal decomposition temperature of bio-based polyester elastomers is generally low, limiting the application of bio-based elastomers. An effective strategy to increase the intrinsic thermal decomposition temperature () of bio-based elastomers is to increase the length of the monomer carbon chain in the bio-based elastomers. In this work, the content of dodecanedioic acid (DDA) in a bio-based polyester elastomer composed of butanediol (BDO) and succinic acid (SUA) was increased to improve the of the bio-based polyester elastomer through the reaction force-field molecular dynamics (ReaxFF-MD) simulations. And the thermal decomposition mechanism of the bio-based polyester was analyzed in detail. By calculating the change rate of the molecular chain mean square displacement (MSD), it was determined that when the content of DDA was 50%, the of the bio-based elastomer was up to 718 K. By calculating the activation energy of thermal decomposition and further analyzing the thermal decomposition process, it is found that the thermal decomposition of the bio-based polyester elastomer is mainly through breaking the C-O bond in the backbone. This work is expected to provide theoretical guidance for designing and fabricating highly heat-resistant bio-based elastomers by systematically exploring the thermal decomposition mechanism of bio-based polyester elastomers.
近年来，由于生物基聚酯弹性体的单体来源广泛且具有环境友好特性，研究人员对其进行了广泛研究。然而，与传统的石油基弹性体相比，生物基聚酯弹性体的热分解温度普遍较低，这限制了生物基弹性体的应用。提高生物基弹性体固有热分解温度（）的一种有效策略是增加生物基弹性体中单体碳链的长度。在这项工作中，通过反应力场分子动力学（ReaxFF-MD）模拟，增加了由丁二醇（BDO）和琥珀酸（SUA）组成的生物基聚酯弹性体中十二烷二酸（DDA）的含量，以提高生物基聚酯弹性体的。并详细分析了生物基聚酯的热分解机理。通过计算分子链均方位移（MSD）的变化率，确定当DDA含量为50%时，生物基弹性体的达到718 K。通过计算热分解活化能并进一步分析热分解过程，发现生物基聚酯弹性体的热分解主要是通过断裂主链中的C-O键。这项工作有望通过系统探索生物基聚酯弹性体的热分解机理，为设计和制备高耐热性生物基弹性体提供理论指导。
