FORTH/IESL and Department of Materials Science and Technology, University of Crete, 71110 Heraklion, Greece.
Soft Matter. 2015 Jun 21;11(23):4640-8. doi: 10.1039/c5sm00411j.
Using a powerful combination of experiments and simulations we demonstrate how the microstructure and its time evolution are linked with mechanical properties in a frustrated, out-of-equilibrium, particle gel under shear. An intermediate volume fraction colloid-polymer gel is used as a model system, allowing quantification of the interplay between interparticle attractions and shear forces. Rheometry, confocal microscopy and Brownian dynamics reveal that high shear rates, fully breaking the structure, lead after shear cessation to more homogeneous and stronger gels, whereas preshear at low rates creates largely heterogeneous weaker gels with reduced elasticity. We find that in comparison, thermal quenching cannot produce structural inhomogeneities under shear. We argue that external shear has strong implications on routes towards metastable equilibrium, and therefore gelation scenarios. Moreover, these results have strong implications for material design and industrial applications, such as mixing, processing and transport protocols coupled to the properties of the final material.
我们通过强大的实验和模拟组合,展示了在受挫折、非平衡的剪切颗粒凝胶中,微结构及其时间演化如何与机械性能相关联。使用中间体积分数的胶体聚合物凝胶作为模型体系,定量研究了颗粒间吸引力和剪切力之间的相互作用。流变学、共聚焦显微镜和布朗动力学揭示了高剪切速率完全破坏结构,在剪切停止后导致更均匀和更强的凝胶,而在低速率预剪切会产生具有降低的弹性的大的不均匀较弱的凝胶。我们发现,相比之下,热淬火在剪切下不能产生结构不均匀性。我们认为,外部剪切对通向亚稳平衡的途径有很强的影响,因此对凝胶化场景也有很强的影响。此外,这些结果对材料设计和工业应用有重要意义,例如混合、加工和与最终材料性能相关的运输协议。