Kinetically controlled homogenization and transformation of crystalline fiber networks in supramolecular materials

Supramolecular materials with three-dimensional fiber networks have applications in many fields. For these applications, a homogeneous fiber network is essential in order to get the desired performance of a material. However, such a fiber network is hard to obtain, particularly when the crystallization of fiber takes place nonisothermally. In this work, a copolymer is used to kinetically control the nucleation and fiber network formation of a small molecular gelling agent, N-lauroyl-L-glutamic acid di-nbutylamide (GP-1) in benzyl benzoate. The retarded nucleation and enhanced mismatch nucleation of the gelator by the additive leads to the conversion of a mixed fiber network into a homogeneous network consisting of spherulites only. The enhanced structural mismatch of the GP-1 during crystallization is quantitatively characterized using the rheological data. This effect also leads to the transformation of an interconnecting (single) fiber network of GP-1 into a multidomain fiber network in another solvent, isostearyl alcohol. The approach developed is significant to the production of supramolecular materials with homogeneous fiber networks and is convenient to switch a single fiber network to a multidomain network without adjusting the thermodynamic driving force.