Mechanical & Aerospace Engineering, University of Florida, FL-32611, USA.
Soft Matter. 2018 Feb 28;14(9):1559-1570. doi: 10.1039/c7sm01518f.
Micro-scale hydrogel particles, known as microgels, are used in industry to control the rheology of numerous different products, and are also used in experimental research to study the origins of jamming and glassy behavior in soft-sphere model systems. At the macro-scale, the rheological behaviour of densely packed microgels has been thoroughly characterized; at the particle-scale, careful investigations of jamming, yielding, and glassy-dynamics have been performed through experiment, theory, and simulation. However, at low packing fractions near jamming, the connection between microgel yielding phenomena and the physics of their constituent polymer chains has not been made. Here we investigate whether basic polymer physics scaling laws predict macroscopic yielding behaviours in packed microgels. We measure the yield stress and cross-over shear-rate in several different anionic microgel systems prepared at packing fractions just above the jamming transition, and show that our data can be predicted from classic polyelectrolyte physics scaling laws. We find that diffusive relaxations of microgel deformation during particle re-arrangements can predict the shear-rate at which microgels yield, and the elastic stress associated with these particle deformations predict the yield stress.
微凝胶颗粒是一种微观尺度的水凝胶粒子,也被称为微球,在工业中用于控制许多不同产品的流变性能,也在实验研究中用于研究软球模型体系中阻塞和玻璃化行为的起源。在宏观尺度上,已对密集填充的微凝胶的流变行为进行了彻底的描述;在颗粒尺度上,通过实验、理论和模拟对阻塞、屈服和玻璃动力学进行了仔细的研究。然而,在接近阻塞的低堆积分数下,微凝胶屈服现象与组成聚合物链的物理性质之间的联系尚未建立。在这里,我们研究了基本的聚合物物理标度定律是否可以预测堆积微凝胶的宏观屈服行为。我们在几种不同的阴离子微凝胶体系中测量了在刚刚超过阻塞转变的堆积分数下的屈服应力和交叉剪切速率,并表明我们的数据可以从经典的聚电解质物理标度定律中预测。我们发现,在颗粒重新排列过程中微凝胶变形的扩散松弛可以预测微凝胶屈服的剪切速率,并且与这些颗粒变形相关的弹性应力可以预测屈服应力。