论文标题

孔径大小的依赖性和在光滑表面上的水凝胶摩擦缓慢松弛

Pore-size dependence and slow relaxation of hydrogel friction on smooth surfaces

论文作者

Cuccia, Nicholas L., Pothineni, Suraj, Wu, Brady, Méndez-Harper, Joshua, Burton, Justin C.

论文摘要

水凝胶由与溶剂(如水分位的水)相互交联的聚合物基质组成,该溶剂的体积分数可能超过90 \%。由于它们可调的生理学特性,生物兼容性和超低摩擦,它们在许多科学和工程应用中都很重要。它们的多相结构导致了复杂的界面流变学,但仍在出现对水凝胶摩擦的详细的微观理解。在这里,我们使用定制的摩擦仪,在这里确定了多丙烯酸(PAA),聚丙烯酰胺(PAAM)和琼脂糖水凝胶球的三种不同的摩擦行为方案。我们发现,在低速度下,摩擦是通过多孔水凝胶网络的流体动力流控制的,并且与特征性孔径成反比。在高速度下,服从弹性水力学理论的凝胶和表面之间形成了一种介质的润滑液膜。在这些机制之间,摩擦力减少了数量级,并在几分钟内显示出缓慢的放松。我们的结果可以解释为聚合物的界面剪切变薄,由于缠绕纠缠而增加了松弛时间。可以通过改变界面处的溶剂盐浓度,溶剂粘度和滑动几何形状来调节这种过渡。

Hydrogel consists of a crosslinked polymer matrix imbibed with a solvent such as water at volume fractions that can exceed 90\%. They are important in many scientific and engineering applications due to their tunable physiochemical properties, bio-compatibility, and ultra-low friction. Their multiphase structure leads to a complex interfacial rheology, yet a detailed, microscopic understanding of hydrogel friction is still emerging. Using a custom-built tribometer, here we identify three distinct regimes of frictional behavior for polyacrylic acid (PAA), polyacrylamide (PAAm), and agarose hydrogel spheres on smooth surfaces. We find that at low velocities, friction is controlled by hydrodynamic flow through the porous hydrogel network, and is inversely proportional to the characteristic pore size. At high velocities, a mesoscopic, lubricating liquid film forms between the gel and surface that obeys elastohydrodynamic theory. Between these regimes, the frictional force decreases by an order of magnitude and displays slow relaxation over several minutes. Our results can be interpreted as an interfacial shear thinning of the polymers with an increasing relaxation time due to the confinement of entanglements. This transition can be tuned by varying the solvent salt concentration, solvent viscosity, and sliding geometry at the interface.

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