Lee Yu-Fan, Chang Wen-Chun, Wu Yvonne, Fan Leia, Lee Eric
Department of Chemical Engineering, National Taiwan University, Taipei 10617, Taiwan.
Langmuir. 2021 Feb 2;37(4):1480-1492. doi: 10.1021/acs.langmuir.0c03002. Epub 2021 Jan 15.
Diffusiophoresis of a soft particle suspended in an infinite medium of symmetric binary electrolyte solution is investigated theoretically in this study, focusing on the chemiphoresis component when there is no global diffusion potential in the bulk solution. The general governing electrokinetic equations are solved with a pseudo-spectral method based on Chebyshev polynomials, and particle mobility, defined as the particle velocity per unit concentration gradient, is calculated. Parameters of electrokinetic interest are examined, in general, to explore their respective impact upon particle motion, such as the fixed charge density and permeability in the outer porous layer, the surface charge density and size of the inner rigid core, and the electrolyte strength in the solution. Nonlinear phenomena such as the motion-deterring double-layer polarization and the counterion condensation effects are scrutinized, in particular, for highly charged soft particles. Mobility reversal is observed in some range of electrolyte strength for highly charged particles. The generation of an axisymmetric counterclockwise vortex flow across the porous layer is found to be responsible for it. The onset of the mobility reversal is synchronized with the appearance or disappearance of this vortex flow. Mobility reversal may happen more than once, with particle moving toward or away from the region of higher solute concentration. The latter is undesirable in the application of drug delivery and thus should be avoided by delicate control of the electrokinetic environment. A local micro diffusion potential is discovered, which always speeds up the migration of coions and slows down that of counterions to guarantee that there is no net electric current across the double layer. Moreover, multilayer structure of the double-layer polarization is discovered when the electrolyte strength is high. The study presented here provides insight and crucial information for practical applications of soft particles, such as drug delivery.
本研究从理论上研究了悬浮在对称二元电解质溶液无限介质中的软颗粒的扩散泳,重点关注本体溶液中不存在全局扩散电位时的化学泳成分。基于切比雪夫多项式的伪谱方法求解了一般的主导电动方程,并计算了定义为单位浓度梯度下颗粒速度的颗粒迁移率。一般来说,研究了电动学相关参数,以探讨它们对颗粒运动的各自影响,例如外多孔层中的固定电荷密度和渗透率、内刚性核的表面电荷密度和尺寸以及溶液中的电解质强度。特别针对高电荷软颗粒仔细研究了诸如阻碍运动的双层极化和反离子凝聚效应等非线性现象。在某些电解质强度范围内,高电荷颗粒会出现迁移率反转现象。发现穿过多孔层产生的轴对称逆时针涡旋流是导致这种现象的原因。迁移率反转的起始与这种涡旋流的出现或消失同步。迁移率反转可能会发生不止一次,颗粒会朝着或远离溶质浓度较高的区域移动。后者在药物递送应用中是不可取的,因此应通过精细控制电动环境来避免。发现了局部微扩散电位,它总是加速同离子的迁移并减缓反离子的迁移,以确保双层中没有净电流。此外,当电解质强度较高时,发现了双层极化的多层结构。本文提出的研究为软颗粒在药物递送等实际应用中提供了见解和关键信息。