Self-Assembled Fullerene Nanostructures for Mimicking and Understanding of Natural Enzymes

Abstract

Self-assembling enzyme mimics offer an easy way to imitate activities of natural enzymes but have not been thus far used to understand the effect of different amino acids on the catalytic activity and why they are evolutionarily preserved for specific catalytic roles. Here, we demonstrated that fullerene nanostructures functionalized with catalytically active amino acids, which form multiple active sites via the self-assembly process in the aqueous environment, serve as an effective system to distinguish the catalytic activity differences resulting from single amino acid changes. A nano-level tuning of intermolecular and intramolecular interactions enabled formation of efficient enzyme mimics. Furthermore, using the carboxyl–imidazole couple found in quite different enzymes as the main catalytic unit, we could mimic different enzyme classes, like hydrolases and lyases, with significant catalytic activities. These designed nanocatalysts were also reusable and catalytically active under physiological conditions like natural enzymes.