Enzyme‐Driven, Switchable Catalysis Based on Dynamic Self‐Assembly of Peptides

Author:

Li Qing1ORCID,Min Jiwei1,Zhang Jiaxing1,Reches Meital2,Shen Yuhe1,Su Rongxin134ORCID,Wang Yuefei14ORCID,Qi Wei134ORCID

Affiliation:

1. State Key Laboratory of Chemical Engineering School of Chemical Engineering and Technology Tianjin University Tianjin 300072 P. R. China

2. Institute of Chemistry The Hebrew University of Jerusalem Jerusalem 91904 Israel

3. Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin 300072 P. R. China

4. Tianjin Key Laboratory of Membrane Science and Desalination Technology Tianjin University Tianjin 300072 P. R. China

Abstract

AbstractCovalent regulatory systems of enzymes are widely used to modulate biological enzyme activities. Inspired by the regulation of reactive‐site phosphorylation in organisms, we developed peptide‐based catecholase mimetics with switchable catalytic activity and high selectivity through the co‐assembly of nanofibers comprising peptides and copper ions (Cu2+). Through careful design and modification of the peptide backbone structure based on the change in the free energy of the system, we identified the peptide with the most effective reversible catalytic activity. Kinase/phosphatase switches were used to control the reversible transition of nanofiber formation and depolymerization, as well as to modulate the active‐site microenvironment. Notably, the self‐assembly and disassembly processes of nanofibers were simulated using coarse‐grained molecular dynamics. Furthermore, theoretical calculations confirmed the coordination of the peptide and Cu2+, forming a zipper‐like four‐ligand structure at the catalytically active center of the nanofibers. Additionally, we conducted a comprehensive analysis of the catalytic mechanism. This study opens novel avenues for designing biomimetic enzymes with ordered structures and dynamic catalytic activities.

Funder

National Natural Science Foundation of China

State Key Laboratory of Chemical Engineering

Seed Foundation of Tianjin University

Publisher

Wiley

Subject

General Chemistry,Catalysis

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