Thermal degradation of butadiene‐based model elastomers was analyzed via a novel reactive molecular dynamics simulation (ReaxFF) method. The molecular simulation was carried out on 40 monomer units connected together. Degradation pathways of both homopolymer and copolymer of butadiene‐based model elastomers such as polybutadiene (BR) and poly (styrene‐co‐butadiene) (SBR) were studied. The evolution of different fragmented products was examined as a function of time and heating rate. The formation mechanisms of different degraded fragments were visualized via the simulation method. The major decomposition products obtained from these model compounds were the monomers and comonomers. Pyrolysis gas chromatography–mass spectrometry (py‐GC–MS) analysis was performed on the commercial samples of BR and SBR to verify the simulation results. The results obtained from the reactive simulation were very consistent with the experimental results. The activation energy required for the thermal decomposition of butadiene‐based model elastomers were calculated both from the ReaxFF simulation and thermogravimetric analysis (TGA). The results were also in good agreement. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020, 137, 48592.

中文翻译：

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反应分子动力学模拟对丁二烯基模型弹性体的高温降解

通过新型反应分子动力学模拟（ReaxFF）方法分析了基于丁二烯的模型弹性体的热降解。在连接在一起的40个单体单元上进行了分子模拟。研究了丁二烯基模型弹性体（如聚丁二烯（BR）和聚（苯乙烯-共丁二烯）（SBR））的均聚物和共聚物的降解途径。检查了不同碎片产品的演变随时间和加热速率的变化。通过模拟方法观察了不同降解片段的形成机理。从这些模型化合物获得的主要分解产物是单体和共聚单体。对商业化的BR和SBR样品进行了热解气相色谱-质谱（py-GC-MS）分析，以验证模拟结果。从反应模拟获得的结果与实验结果非常吻合。通过ReaxFF模拟和热重分析（TGA）计算出丁二烯基模型弹性体热分解所需的活化能。结果也很一致。分级为4 +©2019 Wiley Periodicals，Inc.J.Appl。Polym。科学2020，137，48592。