van der Naald Mike, Zhao Liang, Jackson Grayson L, Jaeger Heinrich M
James Franck Institute and Department of Physics, University of Chicago, Chicago, Illinois, USA.
Soft Matter. 2021 Mar 21;17(11):3144-3152. doi: 10.1039/d0sm01350a. Epub 2021 Feb 18.
The application of stress can drive a dense suspension into a regime of highly non-Newtonian response, characterized by discontinuous shear thickening (DST) and potentially shear jamming (SJ), due to the formation of a frictionally stabilized contact network. Investigating how the molecular weight of the suspending solvent affects the frictional particle-particle interactions, we report on experiments with suspensions of fumed silica particles in polyethylene glycol (PEG). Focusing on the monomer-to-oligomer limit, with n = 1 to 8 ethylene oxide repeat units, we find that increasing n enhances shear thickening under steady-state shear and even elicits rapidly propagating shear jamming fronts, as assessed by high-speed ultrasound imaging of impact experiments. We associate this behavior with a weakening of the solvation layers surrounding the particles as n is increased, which thereby facilitates the formation of frictional contacts. We argue that for n larger than the monomer-to-oligomer limit the trend reverses and frictional interactions are diminished, as observed in prior experiments. This reversal occurs because the polymeric solvent transitions from being enthalpically bound to entropically bound to the particle surfaces, which strengthens solvation layers.
施加应力可使浓悬浮液进入高度非牛顿响应状态,其特征为不连续剪切增稠(DST)以及可能的剪切阻塞(SJ),这是由于形成了摩擦稳定的接触网络。通过研究悬浮溶剂的分子量如何影响颗粒间的摩擦相互作用,我们报告了关于气相二氧化硅颗粒在聚乙二醇(PEG)中的悬浮液实验。聚焦于单体到低聚物的范围,其中环氧乙烷重复单元数(n = 1)至(8),我们发现随着(n)增加,稳态剪切下的剪切增稠增强,甚至通过冲击实验的高速超声成像评估发现会引发快速传播的剪切阻塞前沿。我们将这种行为与随着(n)增加颗粒周围溶剂化层的减弱联系起来,这从而促进了摩擦接触的形成。我们认为,如先前实验所观察到的,当(n)大于单体到低聚物的范围时,趋势会反转,摩擦相互作用会减弱。这种反转的发生是因为聚合物溶剂从与颗粒表面以焓键结合转变为以熵键结合,这增强了溶剂化层。