Hitimana Emmanuel, Roopnarine Brittany K, Morozova Svetlana
Department of Macromolecular Science and Engineering, Case Western Reserve University, Cleveland, OH, USA.
Soft Matter. 2022 Jan 26;18(4):832-840. doi: 10.1039/d1sm01554k.
Transport through heterogeneous confined geometries is encountered in many processes and applications such as filtration, drug delivery, and enhanced oil recovery. We have used differential dynamic microscopy (DDM) and particle tracking to investigate dynamics of 36 nm negatively-charged polystyrene particles in convex lens-induced confinement (CLiC). The confinement gap height was controlled from 0.085 μm to 3.6 mm by sandwiching the aqueous particle solution between a glass coverslip and a convex lens using a homemade sample holder. With an inverted fluorescence microscope, sequences of micrographs were taken at various radial positions and gap heights for five particle concentrations ( = 0.5 × 10, 1 × 10, 5 × 10, 10 × 10, 50 × 10) and ionic strengths ranging from 10 to 150 mM. The resulting image structure functions were fitted with a simple exponential model to extract the ensemble-averaged diffusive dynamics. It was found that particle diffusion was more hindered as a function of increased confinement. In addition, the ensemble-averaged diffusion coefficient was found to depend on the bulk concentration, and the concentration dependence increased as a function of confinement. Increasing particle and salt concentration led to confinement-dependent adsorption onto the geometry surface. Overall, we show that CLiC devices are simple and effective and can be used to study dynamics in continuous confinement from sub 100 nm to 100's of μm. These findings could lead to better understanding of separations and interactions in confining devices.
在许多过程和应用中,如过滤、药物递送和强化采油,都会遇到通过非均匀受限几何结构的传输。我们使用差分动态显微镜(DDM)和粒子追踪技术,研究了36纳米带负电荷的聚苯乙烯粒子在凸透镜诱导受限(CLiC)中的动力学。通过使用自制样品架将水性粒子溶液夹在玻璃盖玻片和凸透镜之间,将受限间隙高度控制在0.085微米至3.6毫米之间。使用倒置荧光显微镜,在五个粒子浓度( = 0.5×10、1×10、5×10、10×10、50×10)和10至150毫摩尔的离子强度下,在不同径向位置和间隙高度拍摄显微照片序列。将所得的图像结构函数用一个简单的指数模型进行拟合,以提取系综平均扩散动力学。结果发现,随着受限程度的增加,粒子扩散受到的阻碍更大。此外,发现系综平均扩散系数取决于本体浓度,并且浓度依赖性随着受限程度的增加而增加。增加粒子和盐的浓度会导致与受限相关的吸附到几何表面上。总体而言,我们表明CLiC装置简单有效,可用于研究从亚100纳米到数百微米的连续受限中的动力学。这些发现有助于更好地理解受限装置中的分离和相互作用。