2026-10-14T20:36:19Z https://api.figshare.com/v2/oai

oai:figshare.com:article/34025049 2026-09-29T16:12:40Z category_1 category_4 category_915 category_14 category_21 category_272 category_873 category_734 category_64 category_135 portal_63 item_type_6 month_year_09_2026

Tuning Hydrogel Mechanics Through Synergistic Metal-Ligand Coordination and Chemical Fueling Chamoni W. H. Rajawasam (14685406) Sophia M. Costantino (25137885) Kavindya. S. J. Ekanayaka (25137888) Jessica L. Sparks (1675408) C. Scott Hartley (1386309) Dominik Konkolewicz (1460365) Biophysics Biochemistry Physical Sciences not elsewhere classified Molecular Biology Biotechnology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified Cancer Computational Biology temporally controllable properties create polymer networks carboxylic acid structure transient mechanical reinforcement transient anhydride formation resulting transient cross tuning hydrogel mechanics yielding materials capable persistent dynamic metal 2 +</ sup transient state programmable mechanics soft materials materials achieve versatile platform synergistic metal supramolecular hydrogels powerful strategy methoxy groups metal ion ligand coordination intrinsic self coordination strength autonomous self 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. 2026-09-29T00:00:00Z Text Journal contribution 10.1021/acspolymersau.6c00161.s001 https://figshare.com/articles/journal_contribution/Tuning_Hydrogel_Mechanics_Through_Synergistic_Metal-Ligand_Coordination_and_Chemical_Fueling/34025049 CC BY-NC 4.0