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Controlling Polymer Morphologies by Intramolecular and Intermolecular Dynamic Covalent Iron(III)/Catechol Complexation—From Polypeptide Single Chain Nanoparticles to Hydrogels
Author(s) -
Hebel Marco,
Gačanin Jasmina,
Lückerath Thorsten,
Ng David Y. W.,
Weil Tanja
Publication year - 2022
Publication title -
macromolecular rapid communications
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.348
H-Index - 154
eISSN - 1521-3927
pISSN - 1022-1336
DOI - 10.1002/marc.202100413
Subject(s) - self healing hydrogels , intermolecular force , intramolecular force , nanoparticle , covalent bond , materials science , catechol , stoichiometry , nanotechnology , polymer , dynamic mechanical analysis , folding (dsp implementation) , chemical engineering , chemistry , polymer chemistry , molecule , organic chemistry , engineering , electrical engineering , composite material
Responsive biomaterials, tunable from the molecular to the macroscopic scale, are attractive for various applications in nanotechnology. Herein, a long polypeptide chain derived from the abundant serum protein human serum albumin is cross‐linked by dynamic‐coordinative iron(III)/catechol bonds. By tuning the binding stoichiometry and the pH, reversible intramolecular folding into polypeptide nanoparticles with controllable sizes is achieved. Moreover, upon varying the stoichiometry, intermolecular cross‐links become predominant yielding smart and tunable macroscopic protein hydrogels. By adjusting the intra‐ and intermolecular interactions, biocompatible and biodegradable materials are formed with varying morphologies and dimensions covering several lengths scales featuring rapid gelation without toxic reagents, fast and autonomous self‐healing, tunable mechanical properties, and high adaptability to local environmental conditions. Such material characteristics can be particularly attractive for tissue engineering approaches to recreate soft tissues matrices with highly customizable features in a fast and simple fashion.