Synthetic Reversible Fibrous Network Hydrogels Based on a Double-Helical Polyelectrolyte
Haonan Zheng1, Kaizheng Liu2, Yongheng Cui1
1State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University 2999 Renmin North Road, Shanghai, 201620, China.
Angewandte Chemie (International Ed. in English)
|March 25, 2025
Summary
Researchers developed the first reversible fibrous network hydrogel using rigid synthetic polyelectrolytes. This novel material exhibits unique thermoreversible gelation and strain-stiffening properties, inspired by biological tissues.
Area of Science:
- Materials Science
- Polymer Chemistry
- Biomaterials Engineering
Background:
- Biological fibrous networks inspire synthetic hydrogels, but reversible formation is challenging.
- Few synthetic polymers can reversibly form fibrous network hydrogels.
Purpose of the Study:
- To report the first reversible fibrous network hydrogel from synthetic polyelectrolytes.
- To investigate the gelation mechanism and properties of this novel hydrogel.
Main Methods:
- Synthesis of double-helical poly(2,2'-disulfonyl-4,4'-benzidine terephthalamide) (PBDT) and tetrabutylphosphonium bromide ([P4444]Br).
- Characterization of the sol-gel transition triggered by temperature and hydrophobicity changes.
- Mechanical testing to evaluate strain-stiffening and hysteresis.
- Investigation of salt effects on the transition temperature.
Main Results:
- A reversible fibrous network hydrogel was formed using rigid PBDT and [P4444]Br.
- The gelation is triggered by the lower critical solution temperature (LCST) of [P4444]Br, leading to PBDT aggregation and network formation.
- The hydrogel exhibits strain-stiffening behavior and significant thermal hysteresis.
- Salt effects on transition temperature deviate from the Hofmeister series, indicating sulfonate group coordination.
Conclusions:
- This study introduces a novel thermoreversible gelation mechanism for rigid polyelectrolytes.
- The developed hydrogel mimics biological mechanical properties and has potential for advanced coatings.
- The findings broaden the scope of synthetic fibrous network hydrogels.
