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稀聚合物溶液在微纳通道中耗尽层与聚合物迁移的耗散粒子动力学模拟

Dissipative particle dynamics simulation of depletion layer and polymer migration in micro- and nanochannels for dilute polymer solutions.

作者信息

Fedosov Dmitry A, Em Karniadakis George, Caswell Bruce

机构信息

Division of Applied Mathematics, Brown University, Providence, Rhode Island 02912, USA.

出版信息

J Chem Phys. 2008 Apr 14;128(14):144903. doi: 10.1063/1.2897761.

Abstract

The flows of dilute polymer solutions in micro- and nanoscale channels are of both fundamental and practical importance in variety of applications in which the channel gap is of the same order as the size of the suspended particles or macromolecules. In such systems depletion layers are observed near solid-fluid interfaces, even in equilibrium, and the imposition of flow results in further cross-stream migration of the particles. In this work we employ dissipative particle dynamics to study depletion and migration in dilute polymer solutions in channels several times larger than the radius of gyration (Rg) of bead-spring chains. We compare depletion layers for different chain models and levels of chain representation, solvent quality, and relative wall-solvent-polymer interactions. By suitable scaling the simulated depletion layers compare well with the asymptotic lattice theory solution of depletion near a repulsive wall. In Poiseuille flow, polymer migration across the streamlines increases with the Peclet and the Reynolds number until the center-of-mass distribution develops two symmetric off-center peaks which identify the preferred chain positions across the channel. These appear to be governed by the balance of wall-chain repulsive interactions and an off-center driving force of the type known as the Segre-Silberberg effect.

摘要

在各种应用中,当通道间隙与悬浮颗粒或大分子的尺寸处于同一数量级时,稀聚合物溶液在微纳尺度通道中的流动具有重要的基础意义和实际意义。在这样的系统中,即使在平衡状态下,在固液界面附近也会观察到耗尽层,而施加流动会导致颗粒进一步的横向迁移。在这项工作中,我们采用耗散粒子动力学来研究比珠簧链回转半径(Rg)大几倍的通道中稀聚合物溶液的耗尽和迁移现象。我们比较了不同链模型、链表示水平、溶剂质量以及相对壁 - 溶剂 - 聚合物相互作用下的耗尽层情况。通过适当的标度,模拟得到的耗尽层与排斥壁附近耗尽的渐近晶格理论解吻合得很好。在泊肃叶流中,聚合物跨流线的迁移随着佩克莱数和雷诺数的增加而增加,直到质心分布形成两个对称的偏心峰,这些峰确定了通道中链的优选位置。这些似乎由壁 - 链排斥相互作用与一种称为塞格雷 - 西尔伯格效应的偏心驱动力之间的平衡所控制。

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