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Abstract The design of hydrogels where multiple interpenetrating networks enable enhanced mechanical properties can broaden their field of application in biomedical materials, 3D printing, and soft robotics. We report a class of self-reinforced homocomposite hydrogels (HHGs) comprised of interpenetrating networks of multiscale hierarchy. A molecular alginate gel is reinforced by a colloidal network of hierarchically branched alginate soft dendritic colloids (SDCs). The reinforcement of the molecular gel with the nanofibrillar SDC network of the same biopolymer results in a remarkable increase of the HHG’s mechanical properties. The viscoelastic HHGs show >3× larger storage modulus and >4× larger Young’s modulus than either constitutive network at the same concentration. Such synergistically enforced colloidal-molecular HHGs open up numerous opportunities for formulation of biocompatible gels with robust structure-property relationships. Balance of the ratio of their precursors facilitates precise control of the yield stress and rate of self-reinforcement, enabling efficient extrusion 3D printing of HHGs.
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Surpassing the strength of metallogels with a rigid, amorphous metal-rich material formulation
Metal-ion-containing soft materials include metallogels, metal-organic frameworks, and coordination polymers. These materials show commercial value in catalysis, hydrogen storage, and electronics. Metal-containing soft materials reported to date are structurally weak, falling short of a Young’s modulus typical of engineering-grade materials. We report herein that inclusion of an antisolvent in metal-thiolate metallogel synthesis results in a colloidal sol, where the colloids comprise amorphous metal-organic complexes. Upon desolvation, the colloids coalesce to form a solid phase that is both gel like and glass like. This solid phase is structurally amorphous, comprises continuous networks similar to organic polymers, and has stiffness observed in polymeric materials with extended structure, yet contains a superstoichiometric amount of metal relative to organic ligand. The solid phase is therefore a rigid, amorphous metal-rich (RAMETRIC) material. Highlighting the rigidity, the Young’s modulus of the gel-phase material is 1,000× greater than metallogels comprised of the same constituent building blocks.
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- Award ID(s):
- 2204110
- PAR ID:
- 10550443
- Publisher / Repository:
- Cell Press
- Date Published:
- Journal Name:
- Cell Reports Physical Science
- Volume:
- 4
- Issue:
- 12
- ISSN:
- 2666-3864
- Page Range / eLocation ID:
- 101738
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1016/j.xcrp.2023.101738
