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Self-Assembly of pH-Responsive Star-Shaped Amphiphilic Polypeptides Based on L-Lysine and L-Leucine

Full text
Author(s):
da Silva, Daniel Jose ; Mendes Cobe, Gabriella ; Colonese Vlasman, Raphael ; Catalani, Luiz Henrique
Total Authors: 4
Document type: Journal article
Source: ACS POLYMERS AU; v. N/A, p. 12-pg., 2025-10-22.
Abstract

Polypeptides are attractive, renewable, and biocompatible materials for broad potential biomedical, pharmaceutical, and regenerative medicine applications. In this study, star-shaped 3-arm amphiphilic polypeptides with self-assembly characteristics were synthesized by ring-opening polymerization (ROP) of N-carboxyanhydride (NCA), incorporating L-leucine and L-lysine to form a core-shell structure. These polymers were thoroughly characterized through various techniques, revealing that their rheological behavior and self-assembly are influenced by factors such as the length of the star-shaped arms, the proportion of hydrophobic amino acids, and the surrounding pH. The synthesized polypeptides can self-assemble into five distinct secondary structures, mimicking natural proteins. Our findings evidence that the design of the block size of the hydrophilic L-lysine core and hydrophobic L-leucine shell shapes the ability to form a physical hydrogel, exhibiting shear-thinning rheological characteristics and a rapid mechanical response. The internal microstructure of the hydrogel is based on a supramolecular self-assembly structure consisting of highly connected nanofibrils. (AU)

FAPESP's process: 20/15986-2 - Synthesis and characterization of photocrosslinkable and functionalizable polypeptides for 3D print
Grantee:Raphael Colonese Vlasman
Support Opportunities: Scholarships in Brazil - Doctorate (Direct)
FAPESP's process: 18/13492-2 - Synthetic and natural scaffolds applied to regenerative medicine
Grantee:Luiz Henrique Catalani
Support Opportunities: Research Projects - Thematic Grants
FAPESP's process: 22/16427-2 - Photo-crosslinkable N-carboxyanhydride derived polypeptides with pseudoplastic characteristics for extrusion-based 3D printing
Grantee:Daniel José da Silva
Support Opportunities: Scholarships in Brazil - Post-Doctoral