Self-Sorting Double-Network Hydrogels with Tunable Supramolecular Handedness and Mechanical Properties

Area of Science:

• Supramolecular Chemistry
• Materials Science
• Chiral Materials

Background:

• Biological self-assembly exhibits complex behaviors like self-sorting, which are challenging to replicate in artificial systems.
• Achieving orthogonal and simultaneous operations in synthetic self-assembly remains a significant hurdle.

Purpose of the Study:

• To design and synthesize two distinct gelators capable of forming hydrogels with opposite supramolecular handedness.
• To investigate the spontaneous self-sorting and organization of these gelators into double-network nanofibers.
• To explore the tunability of chiroptical properties and mechanical enhancements in the resulting composite hydrogels.

Main Methods:

• Design of two gelators (LPF and LPFEG) with a common chiral core and differing peripheral substituents.
• Formation of hydrogels with opposite supramolecular handedness from individual gelators.
• Mixing of the two hydrogels to induce spontaneous self-sorting and formation of double-network nanofibers.
• Characterization of chiroptical activity and mechanical properties (storage and loss modulus) of the composite hydrogels.

Main Results:

• Successful synthesis of two gelators leading to hydrogels with opposite supramolecular handedness.
• Observation of spontaneous self-sorting and formation of double-network nanofibers upon mixing the hydrogels.
• Demonstration of tunable chiroptical activity by varying the molar ratio of the two gelators.
• Significant enhancement in mechanical properties (storage and loss modulus) observed in the double-network hydrogels, particularly at a 3:7 LPF/LPFEG ratio.

Conclusions:

• The designed gelators enable unprecedented self-sorting and orthogonal self-assembly in artificial systems.
• The resulting double-network hydrogels exhibit tunable chiroptical properties and significantly improved mechanical strength.
• This work provides a novel platform for developing advanced functional materials through controlled supramolecular organization.