Pyell Ute
Department of Chemistry, University of Marburg, Marburg, Germany.
Electrophoresis. 2008 Feb;29(3):576-89. doi: 10.1002/elps.200700411.
The electrophoretic mobility of silica-encapsulated semiconductor nanocrystals (quantum dots) dependent on the pH and the ionic strength of the separation electrolyte has been determined by CE. Having shown the viability of the approach, the electrophoretic mobility mu of the nanoparticles investigated is calculated for varied zeta potential zeta, particle radius r, and ionic strength I employing an approximate analytical expression presented by Ohshima (J. Colloid Interface Sci. 2001, 239, 587-590). The comparison of calculated with measured data shows that the experimental observations exactly follow what would be expected from theory. Within the parameter range investigated at fixed zeta and I there is an increase in mu with r which is a nonlinear function. This dependence of mu on size parameters can be used for the size-dependent separation of particles. Modeling of mu as function of I and zeta makes it possible to calculate the size distribution of nanoparticles from electrophoretic data (using the peak shape of the particle zone in the electropherogram) without the need for calibration provided that zeta is known with adequate accuracy. Comparison of size distributions calculated via the presented method with size histograms determined from transmission electron microscopy (TEM) micrographs reveals that there is an excellent matching of the size distribution curves obtained with the two independent methods. A comparison of calculated with measured distributions of the electrophoretic mobility showed that the observed broad bands in CE studies of colloidal nanoparticles are mainly due to electrophoretic heterogeneity resulting from the particle size distribution.
通过毛细管电泳(CE)测定了二氧化硅包覆的半导体纳米晶体(量子点)的电泳迁移率,该迁移率取决于分离电解质的pH值和离子强度。在证明了该方法的可行性之后,利用大岛(Ohshima)提出的近似解析表达式(《胶体与界面科学杂志》,2001年,第239卷,第587 - 590页),针对不同的zeta电位ζ、颗粒半径r和离子强度I,计算了所研究纳米颗粒的电泳迁移率μ。计算数据与测量数据的比较表明,实验观察结果完全符合理论预期。在固定ζ和I的研究参数范围内,μ随r增加,且呈非线性函数关系。μ对尺寸参数的这种依赖性可用于颗粒的尺寸依赖性分离。将μ建模为I和ζ的函数,使得在已知ζ具有足够精度的情况下,无需校准即可根据电泳数据(利用电泳图中颗粒区的峰形)计算纳米颗粒的尺寸分布。通过本文提出的方法计算得到的尺寸分布与通过透射电子显微镜(TEM)显微照片确定的尺寸直方图的比较表明,两种独立方法得到的尺寸分布曲线匹配良好。计算得到的电泳迁移率分布与测量分布的比较表明,在胶体纳米颗粒的CE研究中观察到的宽带主要是由于颗粒尺寸分布导致的电泳异质性。