Department of Physics and Astronomy, University of California, Irvine, California 92697, United States.
ACS Nano. 2013 Apr 23;7(4):3720-8. doi: 10.1021/nn400774e. Epub 2013 Apr 5.
In this article, we report detection of deformable, hydrogel particles by the resistive-pulse technique using single pores in a polymer film. The hydrogels pass through the pores by electroosmosis and cause formation of a characteristic shape of resistive pulses indicating the particles underwent dehydration and deformation. These effects were explained via a non-homogeneous pressure distribution along the pore axis modeled by the coupled Poisson-Nernst-Planck and Navier-Stokes equations. The local pressure drops are induced by the electroosmotic fluid flow. Our experiments also revealed the importance of concentration polarization in the detection of hydrogels. Due to the negative charges as well as branched, low-density structure of the hydrogel particles, the concentration of ions in the particles is significantly higher than in the bulk. As a result, when an electric field is applied across the membrane, a depletion zone can be created in the vicinity of the particle observed as a transient drop of the current. Our experiments using pores with openings between 200 and 1600 nm indicated the concentration polarization dominated the hydrogels' detection of pores wider than 450 nm. The results are of importance for all studies that involve transport of molecules, particles, and cells through pores with charged walls. The developed inhomogeneous pressure distribution can potentially influence the shape of the transported species. The concentration polarization changes the interpretation of the resistive pulses; the observed current change does not necessarily reflect only the particle size but also the size of the depletion zone that is formed in the particle vicinity.
在本文中,我们报告了使用聚合物膜中的单个孔通过电阻脉冲技术检测可变形水凝胶颗粒。水凝胶通过电渗通过孔,并导致形成指示颗粒经历脱水和变形的特征形状的电阻脉冲。这些效应通过沿孔轴的非均匀压力分布来解释,该压力分布通过耦合的泊松-纳斯特-普朗克和纳维-斯托克斯方程来建模。局部压降由电渗流引起。我们的实验还揭示了浓度极化在水凝胶检测中的重要性。由于水凝胶颗粒带有负电荷和支化的低密度结构,颗粒中的离子浓度明显高于本体。因此,当电场跨膜施加时,在颗粒附近可以创建耗尽区,观察到电流的瞬态下降。我们使用开口在 200 和 1600nm 之间的孔进行的实验表明,当孔宽大于 450nm 时,浓度极化主导了水凝胶对孔的检测。对于所有涉及带电荷壁的分子、颗粒和细胞通过孔的传输的研究,这些结果都很重要。所开发的非均匀压力分布可能会影响传输物质的形状。浓度极化改变了对电阻脉冲的解释;观察到的电流变化不一定仅反映颗粒尺寸,还反映在颗粒附近形成的耗尽区的尺寸。