Nucleophilic Regulation of the Formation of Melanin-like Species by Amyloid Fibers

[Image: see text] This work examines the influences of amyloid fibers of hen egg white lysozyme (HEWL) on the formation of melanin-like species (MLS) with a rationally selected set of catechol derivatives. Catechol–amyloid interactions, which are central in melanogenesis, are complex and multifaceted, making them difficult to understand at the molecular level. The catechol derivatives are set to interact with HEWL amyloid fibers upon altering pH, and the resultant formation of MLS is characterized. For obtaining clues for the molecular mechanism by which HEWL fibers regulate the formation of MLS, putative intermolecular interactions are individually perturbed and their ramifications are analyzed. With the entire data set, we could conclude that the externally presented nucleophilic moieties of HEWL fibers play a major role in regulating the material and kinetic properties of MLS and their formation, respectively.