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Printing Double-Network Tough Hydrogels Using Temperature-Controlled Projection Stereolithography (TOPS)
Puskal Kunwar1,2, Bianca Louise Andrada1,2, Arun Poudel1,2
1Biomedical and Chemical Engineering Department, Syracuse University, Syracuse, New York 13210, United States.
ACS Applied Materials & Interfaces
|June 15, 2023
Summary
We developed a new method to 3D print tough double-network (DN) hydrogels with superior mechanical properties. This technique enables the creation of custom, mechanically reconfigurable flexible devices like tunable lenses.
Area of Science:
- Materials Science
- Polymer Chemistry
- Biomaterials
Background:
- Double-network (DN) hydrogels offer enhanced mechanical properties but are challenging to fabricate into complex 3D structures.
- Existing methods often lack the resolution or material versatility for advanced applications.
Purpose of the Study:
- To develop a novel method for fabricating 3D customized double-network (DN) hydrogel structures.
- To achieve superior mechanical performance in both tension and compression for printed hydrogels.
- To demonstrate the potential for creating mechanically reconfigurable devices.
Main Methods:
- Optimized a one-pot prepolymer formulation with photo-cross-linkable acrylamide and thermoreversible κ-carrageenan.
- Utilized a 3D printing system (TOPS) to photopolymerize the acrylamide network above the κ-carrageenan sol-gel transition temperature.
- Generated the secondary κ-carrageenan network via cooling to create tough DN hydrogels.
Main Results:
- Achieved high printing resolutions (37 μm lateral, 180 μm vertical) and design freedom (internal voids).
- Demonstrated exceptional mechanical properties: 200 kPa ultimate tensile stress at 2400% strain, and 15 MPa compressive stress at 95% strain, with high recovery.
- Investigated the influence of swelling, necking, self-healing, dehydration, and rehydration on mechanical behavior.
- Successfully printed a functional axicon lens, demonstrating dynamic Bessel beam tuning via tensile stretching.
Conclusions:
- The developed method enables the fabrication of complex 3D DN hydrogels with outstanding and tunable mechanical properties.
- This technology facilitates the creation of novel, mechanically reconfigurable smart devices for diverse applications.
- The technique is broadly applicable to other hydrogel systems for advanced material development.

