Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technische Universität Darmstadt, Alarich-Weiss-Street 8, 64287 Darmstadt, Germany.
Department of Mechanical Engineering, National Institute of Technology Warangal, Warangal, 506004 Telangana, India.
J Chem Theory Comput. 2021 Jun 8;17(6):3772-3782. doi: 10.1021/acs.jctc.1c00134. Epub 2021 May 5.
Polymer sequence engineering is emerging as a potential tool to modulate material properties. Here, we employ a combination of a genetic algorithm (GA) and atomistic molecular dynamics (MD) simulation to design polyethylene-polypropylene (PE-PP) copolymers with the aim of identifying a specific sequence with high thermal conductivity. PE-PP copolymers with various sequences at the same monomer ratio are found to have a broad distribution of thermal conductivities. This indicates that the monomer sequence has a crucial effect on thermal energy transport of the copolymers. A non-periodic and non-intuitive optimal sequence is indeed identified by the GA, which gives the highest thermal conductivity compared with any regular block copolymers, for example, diblock, triblock, and hexablock. In comparison to the bulk density, chain conformations, and vibrational density of states, the monomer sequence has the strongest impact on the efficiency of thermal energy transport via inter- and intra-molecular interactions. Our work highlights polymer sequence engineering as a promising approach for tuning the thermal conductivity of copolymers, and it provides an example application of integrating atomistic MD modeling with the GA for computational material design.
聚合物序列工程正在成为一种调节材料性能的潜在工具。在这里，我们采用遗传算法（GA）和原子分子动力学（MD）模拟的组合，设计具有高导热系数的聚乙烯-聚丙烯（PE-PP）共聚物，目的是确定具有特定序列的共聚物。在相同单体比的情况下，具有不同序列的 PE-PP 共聚物具有广泛的导热系数分布。这表明单体序列对共聚物的热能传递有至关重要的影响。GA 确实确定了一个非周期性和非直观的最佳序列，与任何规则嵌段共聚物（例如二嵌段、三嵌段和六嵌段）相比，该序列具有最高的导热系数。与体密度、链构象和振动态密度相比，单体序列通过分子间和分子内相互作用对热能传递效率的影响最大。我们的工作强调了聚合物序列工程作为调节共聚物导热系数的一种很有前途的方法，并提供了一个将原子 MD 建模与 GA 集成用于计算材料设计的示例应用。
