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Solvent-Driven Biphasic Architectures in Polymer Gels via Polymerization-Induced Solvent Phase Separation.

Yuji Kamiyama¹, Ryota Tamate¹

¹Research Center for Macromolecules & Biomaterials, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba 305-0047, Japan.

Journal of the American Chemical Society

|July 2, 2026

Summary

We developed polymerization-induced solvent phase separation (PI-SPS) to create versatile biphasic polymer gels. This novel method enhances mechanical properties like self-healing and crack resistance for advanced soft materials.

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Area of Science:

Materials Science
Polymer Chemistry
Soft Matter Physics

Background:

Biphasic polymer gels offer advanced functionalities like improved mechanical strength and controlled drug delivery.
Traditional methods for creating biphasic gels are limited in structural diversity and tunability due to monomer copolymerization constraints.

Purpose of the Study:

Introduce a novel, facile, solvent-driven strategy for constructing biphasic polymer gels.
Explore the potential of polymerization-induced solvent phase separation (PI-SPS) for creating tunable soft materials.

Main Methods:

Developed a "polymerization-induced solvent phase separation" (PI-SPS) strategy.
Utilized a homogeneous precursor solution with two immiscible solvents and a monomer.
Triggered solvent demixing during polymerization to form a hierarchical structure.

Main Results:

Achieved biphasic gel formation across diverse solvent systems including water, organic solvents, and ionic liquids.
Demonstrated emergent properties such as self-healing, shape-memory behavior, and enhanced crack resistance (4600 J m^-2).
Hierarchical structures resulted from the spatial organization of solvent domains and polymer networks.

Conclusions:

PI-SPS is a versatile and generalizable strategy for fabricating biphasic soft materials.
The method allows for controlled tuning of solvent affinities to engineer material properties.
This approach opens new avenues for designing advanced functional polymer gels.