Control of crystallization in supramolecular soft materials engineering

As one class of the most important supramolecular functional materials, gels formed by low molecular weight gelators (LMWGs) have many important applications. The key important parameters affecting the in-use performance of a gel are determined by the hierarchical fiber network structures. Fiber networks consisting of weakly interacting multiple domains are commonly observed in gels formed by LMWGs. The rheological properties, particularly the elasticity, of a gel with such a fiber network are weak due to the weak interactions between the individual domains. As achieving desirable rheological properties of such a gel is practically relevant, in this work, we demonstrate the engineering of gels with such a type of fiber network by controlling crystallization of the gelator. Two example gels formed by a glutamic acid derivative in a non-ionic surfactant Tween 80 and in propylene glycol were engineered by controlling the thermodynamic driving force for crystallization. For a fixed gelator concentration, the thermodynamic driving force was manipulated by controlling the temperature for fiber crystallization. It was observed that there exists an optimal temperature at which a gel with maximal elasticity can be fabricated. This will hopefully provide guidelines for producing high performance soft materials by engineering their fiber network structures.