链刚性和剪切场对环形聚合物熔体中纳米颗粒分散和空间分布的影响

Effects of chain stiffness and shear flow on nanoparticle dispersion and distribution in ring polymer melts

目的:一般情况下,纳米粒子在环形聚合物熔体中处于聚集状态。本文通过增加链刚性或施加稳定的剪切场来诱导纳米粒子在环形聚合物熔体中的聚集-分散转变,使环形聚合物中的纳米粒子达到最优的分散状态。创新点:同时改变链刚性和剪切场强度,诱导纳米粒子在分散的同时进行有序排列。方法:利用分子动力学模拟方法,研究纳米粒子在环形聚合物熔体中的分散和空间分布。结论:1.在较弱的高分子/纳米粒子(polymer-NP)相互作用力下,增加环链的刚性或施加剪切场,可以诱导纳米粒子(NPs)从聚集态向分散态过渡。2.增加链的刚性可以提高NPs在环形聚合物熔体中的分散度;NPs被半刚性(或棒状)环形聚合物链包裹,有效地避免了NPs间的聚集,促使其分散。3.随着剪切场强度的增加,聚集的NPs也会因polymer-NP相互作用、NP-NP相互作用以及剪切场之间的竞争而趋于分散;由于polymer-NP相互作用强,所以NPs的空间分布具有良好的有序性和分散性。4.同时考虑剪切场和链刚性,可有效提高NPs在环形聚合物熔体中的分散度和空间分布,而链刚性的增加干扰了NPs的有序结构。

The dispersion behavior and spatial distribution of nanoparticles(NPs)in ring polymer melts are explored by using molecular dynamics(MD)simulations.As polymer-NP interactions increase,three general categories of polymer-mediated NP organization are observed,namely,contact aggregation,bridging,and steric dispersion,consistent with the results of equivalent linear ones in previous studies.In the case of direct contact aggregation among NPs,the explicit aggregation-dispersion transition of NPs in ring polymer melts can be induced by increasing the chain stiffness or applying a steady shear flow.Results further indicate that NPs can achieve an optimal dispersed state with the appropriate chain stiffness and shear flow.Moreover,shear flow cannot only improve the dispersion of NPs in ring polymer melts but also control the spatial distribution of NPs into a well-ordered structure.This improvement becomes more evident under stronger polymer-NP interactions.The observed induced-dispersion or ordered distribution of NPs may provide efficient access to the design and manufacture of high-performance polymer nanocomposites(PNCs).