Dutta Debashis
Department of Chemistry, University of Wyoming, Laramie, WY, 82071, United States.
J Chromatogr A. 2017 Feb 10;1484:85-92. doi: 10.1016/j.chroma.2017.01.004. Epub 2017 Jan 3.
Pressure-driven cross-flows can arise in free-flow isoelectric focusing systems (FFIEF) due to a non-uniform electroosmotic flow velocity along the channel width induced by the pH gradient in this direction. In addition, variations in the channel cross-section as well as unwanted differences in hydrostatic heads at the buffer/sample inlet ports can also lead to such pressure-gradients which besides altering the equilibrium position of the sample zones have a tendency to substantially broaden their widths deteriorating the separations. In this situation, a thorough assessment of stream broadening due to transverse pressure-gradients in FFIEF devices is necessary in order to establish accurate design rules for the assay. The present article describes a mathematical framework to estimate the noted zone dispersion in FFIEF separations based on the method-of-moments approach under laminar flow conditions. A closed-form expression has been derived for the spatial variance of the analyte streams at their equilibrium positions as a function of the various operating parameters governing the assay performance. This expression predicts the normalized stream variance under the chosen conditions to be determined by two dimensionless Péclet numbers evaluated based on the transverse pressure-driven and electrophoretic solute velocities in the separation chamber, respectively. Moreover, the analysis shows that while the stream width can be expected to increase with an increase in the value of the first Péclet number, the opposite trend will be followed with respect to the latter. The noted results have been validated using Monte Carlo simulations that also establish a time/length scale over which the predicted equilibrium stream width is attained in the system.
在自由流动等电聚焦系统(FFIEF)中,由于沿通道宽度方向的pH梯度引起的电渗流速度不均匀,会产生压力驱动的横向流。此外,通道横截面的变化以及缓冲液/样品入口处静水压头的不必要差异也会导致这种压力梯度,这除了会改变样品区的平衡位置外,还会使样品区宽度大幅增加,从而降低分离效果。在这种情况下,有必要对FFIEF装置中横向压力梯度导致的谱带展宽进行全面评估,以便为该分析建立准确的设计规则。本文描述了一个数学框架,用于在层流条件下基于矩量法估计FFIEF分离中上述的谱带扩散。已推导得出分析物流在其平衡位置处的空间方差的闭式表达式,该表达式是控制分析性能的各种操作参数的函数。该表达式预测,在所选条件下,归一化的谱带方差由分别基于分离室中横向压力驱动和电泳溶质速度评估的两个无量纲佩克莱数决定。此外,分析表明,虽然谱带宽度预计会随着第一个佩克莱数的增加而增加,但对于后者则会呈现相反的趋势。上述结果已通过蒙特卡罗模拟得到验证,该模拟还确定了系统达到预测的平衡谱带宽度所需的时间/长度尺度。