ACS Polymers Au· 2026Q1
Tuning Hydrogel Mechanics Through Synergistic Metal-Ligand Coordination and Chemical Fueling
- 0citations
- Q1SCImago
- 2026year
Short summary
Researchers developed metallo-supramolecular hydrogels with two independent crosslinking mechanisms, metal-ligand coordination and transient anhydride formation, enabling programmable stiffness, self-healing, and temporal control.
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Key points
- Hydrogels utilize dual crosslinking: persistent metal-ligand coordination and transient, fuel-driven anhydride formation.
- Stiffness and properties are programmable by tuning metal ions (Fe2+, Ni2+), ligand substituents, and carboxylic acid structures.
- Materials achieve >90% lap-shear healing within 15 hours under fueled conditions.
- Fueling accelerates healing, synergizing with the persistent dynamic crosslinks.
AI-generated from the title and abstract; the full text is not read.
Abstract
Abstract Chemically fueled anhydride formation offers a powerful strategy to create polymer networks with transient mechanical reinforcement. In this work, metallo-supramolecular hydrogels were developed with two independent crosslinking mechanisms, metal-ligand coordination and transient anhydride formation, yielding materials capable of programmable stiffness, intrinsic self-healing, and temporally controllable properties. Bis(pyridin-2-ylmethyl)amine (DPA) units were incorporated into polymers as ligands. The coordination strength of the resulting persistent dynamic cross-links is tunable by varying both the metal ion (Fe2+ or Ni2+) and the nature of the ligands through substitution with chloro or methoxy groups. Carboxylic acid repeat units provide fuel-driven transient anhydride formation on treatment with carbodiimides. The resulting transient cross-links can be tuned by changing the carboxylic acid structure, affecting the lifetime of the transient state and its stiffness. Lap-shear-inspired healing tests show that the materials achieve more than 90% healing under fueled conditions within 15 h. Notably, the fuel-driven process accelerates healing resulting from the persistent dynamic metal-ligand coordination. This work demonstrates a versatile platform for soft materials with programmable mechanics and autonomous self-healing.
The authors' abstract, as published at the source. ACS Polymers Au, 2026 · DOI ↗
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Field: Polymers and Plastics
Polymers and PlasticsMaterials Science