Particle Diffusion in Polymeric Hydrogels with Mixed Attractive and Repulsive Interactions,Nano Letters

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Particle Diffusion in Polymeric Hydrogels with Mixed Attractive and Repulsive Interactions
Nano Letters ( IF 9.6 ) Pub Date : 2018-06-27 00:00:00 , DOI: 10.1021/acs.nanolett.8b02218
Johann Hansing ₁ , Joseph R. Duke ₂ , Emily B. Fryman ₂ , Jason E. DeRouchey ₂ , Roland R. Netz ₁

Affiliation

All biogels are heterogeneous, consisting of functional groups with different biophysical properties arrayed on spatially disordered polymer networks. Nanoparticles diffusing in such biogels experience a mixture of attractive and repulsive interactions. Here, we present experimental and theoretical studies of charged particle diffusion in gels with a random distribution of attractive and repulsive electrostatic interaction sites inside the gel. In addition to interaction disorder, we theoretically investigate the effect of spatial disorder of the polymer network. Our coarse-grained simulations reveal that attractive interactions primarily determine the diffusive behavior of the particles in systems with mixed attractive and repulsive interactions. As a consequence, charged particles of either sign are immobilized in mixed cationic/anionic gels because they are trapped near oppositely charged interaction sites, whereas neutral particles diffuse rapidly. Even small fractions of oppositely charged interaction sites lead to strong trapping of a charged particle. Translational diffusion coefficients of charged probe molecules in gels consisting of mixed cationic and anionic dextran polymers are determined by fluorescence correlation spectroscopy and quantitatively confirm our theoretical predictions.

中文翻译：

具有吸引和排斥相互作用的聚合物水凝胶中的粒子扩散

所有生物凝胶都是异质的，由排列在空间无序的聚合物网络上的具有不同生物物理特性的官能团组成。在这种生物凝胶中扩散的纳米颗粒会经历吸引和排斥相互作用的混合。在这里，我们介绍了带电粒子在凝胶中扩散的实验和理论研究，凝胶内部具有吸引性和排斥性的静电相互作用位点，它们的分布是随机的。除了相互作用紊乱，我们从理论上研究了聚合物网络空间紊乱的影响。我们的粗粒度模拟显示，吸引相互作用主要决定具有吸引和排斥相互作用的系统中粒子的扩散行为。作为结果，任何一个带正负号的粒子都固定在混合的阳离子/阴离子凝胶中，因为它们被困在带相反电荷的相互作用位点附近，而中性粒子则迅速扩散。甚至一小部分带相反电荷的相互作用位点也会导致强烈捕获带电粒子。通过荧光相关光谱法确定了由混合的阳离子和阴离子葡聚糖聚合物组成的凝胶中带电探针分子的平移扩散系数，并定量证实了我们的理论预测。

更新日期：2018-06-27

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