Accelerated ReaxFF Simulations for Describing the Reactive Cross-Linking of Polymers

雷亚克夫 聚合物 力场(虚构) 材料科学 聚合 分子动力学 化学物理 化学 计算化学 计算机科学 有机化学 原子间势 人工智能
作者
Aniruddh Vashisth,Chowdhury Ashraf,Weiwei Zhang,Charles E. Bakis,Adri C. T. van Duin
出处
期刊:Journal of Physical Chemistry A [American Chemical Society]
卷期号:122 (32): 6633-6642 被引量:148
标识
DOI:10.1021/acs.jpca.8b03826
摘要

Various methods have been developed to perform atomistic-scale simulations for the cross-linking of polymers. Most of these methods involve connecting the reactive sites of the monomers, but these typically do not capture the entire reaction process from the reactants to final products through transition states. Experimental time scales for cross-linking reactions in polymers range from minutes to hours, which are time scales that are inaccessible to atomistic-scale simulations. Because simulating reactions on realistic time scales is computationally expensive, in this investigation, an accelerated simulation method was developed within the ReaxFF reactive force field framework. In this method, the reactants are tracked until they reach a nonreactive configuration that provides a good starting point for a reactive event. Subsequently, the reactants are provided with a sufficient amount of energy-equivalent or slightly larger than their lowest-energy reaction barrier-to overcome the barrier for the cross-linking process and form desired products. This allows simulation of cross-linking at realistic, low temperatures, which helps to mimic chemical reactions and avoids unwanted high-temperature side reactions and still allows us to reject high-barrier events. It should be noted that not all accelerated events are successful as high local strain can lead to reaction rejections. The validity of the ReaxFF force field was tested for three different types of transition state, possibly for polymerization of epoxides, and good agreement with quantum mechanical methods was observed. The accelerated method was further implemented to study the cross-linking of diglycidyl ether of bisphenol F (bis F) and diethyltoluenediamine (DETDA), and a reasonably high percentage (82%) of cross-linking was obtained. The simulated cross-linked polymer was then tested for density, glass transition temperature, and modulus and found to be in good agreement with experiments. Results indicate that this newly developed accelerated simulation method in ReaxFF can be a useful tool to perform atomistic-scale simulations on polymerization processes that have a relatively high reaction barrier at a realistic, low temperature.
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