Home > Articles > Published articles > pH-responsive self-assembly of amyloid fibrils for dual hydrolase-oxidase reactions |
Date: | 2021 |
Abstract: | There is an increasing interest in synthetic systems that can execute bioinspired chemical reactions without requiring the complex structures that characterize enzymes in their components. The hierarchical self-assembly of peptides provides a means to create catalytic microenvironments. Ideally, as it occurs in enzymes, the catalytic activity of peptide nanostructures should be reversibly regulated. In a typical enzyme mimetic design, the peptide's self-assembling and catalytic activities are segregated into different regions of the sequence. Here, we aimed to design minimal peptides in which the self-assembly and function were all encoded in the same amino acids. Moreover, we wanted to endow the resulting one-component nanomaterial with divergent, chemically unrelated, catalytic activities, a property not observed in natural enzymes. We show that short peptides consisting only of histidine and tyrosine residues, arranged in a binary pattern, form biocompatible amyloid-like fibrils and hydrogels combining hydrolytic and electrocatalytic activities. The nanofibers' mesoscopic properties are controlled by pH, the transition between assembled active β-sheet fibrils, and disassembled inactive random coil species occurring in a physiologically relevant pH range. The structure of one of such amyloid-like fibrils, as derived from molecular dynamic simulations, provides insights on how they attain this combination of structural and catalytic properties. |
Grants: | Ministerio de Economía y Competitividad BFU2013-44763-P Ministerio de Economía y Competitividad BIO2016-78310-R Ministerio de Educación, Cultura y Deporte FPU14/05786 Agencia Estatal de Investigación CTQ2017-89132-P Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1323 |
Note: | Altres ajuts: ICREA Academia 2015 |
Rights: | Tots els drets reservats. |
Language: | Anglès |
Document: | Article ; recerca ; Versió acceptada per publicar |
Subject: | Amyloid fibrils ; Artificial enzymes ; Hydrogels ; Ph-responsive materials ; Self-assembly ; Short peptides |
Published in: | ACS catalysis, Vol. 11, Issue 2 (January 2021) , p. 595-607, ISSN 2155-5435 |
Postprint 47 p, 5.4 MB |