LLPS-Driven Kinetic Trapping and Thermally Induced Structural Maturation in an Amyloid-Inspired Dipeptide Gel

This is the authors' abstract. We don't add key points for this paper.

Peptide nanoarchitectonics represents the controlled orchestration of dynamic and adaptive bioinspired organized nanostructures for versatile applications. Herein, we investigate the organization of an amyloid-inspired minimalistic dipeptide into diverse nanoarchitectonics. The dipeptide assembled via liquid-liquid phase separation into a kinetically trapped gel state, characterized by the coexistence of gel-like droplets and fibrous domains. This arrested state, upon heating, reached a thermodynamically stable organization with a dense network of thicker fibrils exhibiting improved mechanical properties and increased turbidity. This "thermal bisignate" gel-gel transition depended on the solvent composition; increased DMSO% led to thermoreversible gels showing a gel-sol-gel transition. This hierarchical evolution, spanning droplets and fibrils, exemplifies thermally programmable peptide nanoarchitectonics, offering new avenues to develop amyloid-inspired biomaterials with tunable properties.