Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE 19716, USA.
Theoretical Separation Science Laboratory, Kroungold Analytical Inc., 1299 Butler Pike, Blue Bell, PA 19422, USA.
J Chromatogr A. 2019 Mar 15;1588:85-98. doi: 10.1016/j.chroma.2018.12.040. Epub 2018 Dec 21.
Using random walk techniques, high resolution simulations of zone shape are conducted in open capillary tubes for short and long tube conditions. Finite size solutes are used as tracers in this treatment. Slip flow boundary conditions and wall retention are utilized as needed. These simulations are able to reproduce previous work in short and long tubes. For the short tube case where dispersion does not asymptotically approach the classic Taylor-Aris and Golay solutions, the effect of slip flow boundaries in the transient region shows zone shapes with abbreviated tails where the larger slip flow values cause zone compression. The use of slip flow to lower dispersion in capillary-based, wall-coated separations is shown to favor long tube behavior. This is because slip flow is relevant for cases where slip lengths are fractions of small capillary tube diameters. Incorporating slip flow into transport in capillaries favors a very small capillary radius where the cross-sectional diffusion length is very small and sampling times are fast. The purely convective zone shape with slip flow boundaries is derived analytically. Applications for this type of separation, guided by both analytical theory and simulation, show the potential for nano-sized capillary tubes less than 1 μm in diameter and favor very fast isocratic separations. Using long tube retention theory with slip boundaries shows that the dispersion-reducing region is most important in the range 0 ≤ k' ≤ 1, a relatively small retention window. Further discussion of the gradient elution technique and dispersion in packed beds suggests that the general usage of slip flow boundaries is restricted in liquid phase separation systems.
采用随机游动技术,对开管中短管和长管条件下的区域形状进行了高分辨率模拟。在这种处理中,有限大小的溶质用作示踪剂。需要时使用滑移流边界条件和壁保留。这些模拟能够再现短管和长管中的先前工作。对于短管情况,其中分散作用不会渐近地接近经典的 Taylor-Aris 和 Golay 解,滑移流边界在瞬变区域中的影响显示出具有缩短尾部的区域形状,其中较大的滑移流值导致区域压缩。在基于毛细管的壁涂分离中使用滑移流来降低分散被证明有利于长管行为。这是因为滑移流对于滑移长度是小毛细管直径的分数的情况是相关的。在毛细管中纳入滑移流对传输有利的情况是毛细管半径非常小,其中横截面扩散长度非常小,采样时间非常快。具有滑移流边界的纯对流区域形状是通过解析推导出来的。由分析理论和模拟指导的这种分离类型的应用表明,直径小于 1μm 的纳米级毛细管具有潜力,并且有利于非常快速的等度分离。使用带有滑移边界的长管保留理论表明,在 0≤k'≤1 的范围内,即相对较小的保留窗口,分散减少区域是最重要的。进一步讨论梯度洗脱技术和填充床中的分散作用表明,在液相分离系统中,滑移流边界的一般使用受到限制。