Title:

Designing DNA Intercalating Supramolecular Hydrogels with Tunable Structural Properties

DNA intercalating supramolecular hydrogels (DISHs) are dynamic materials formed through reversible binding of small molecule intercalators to DNA. Intercalation serves as the primary cross-linking mechanism, enabling the formation of 3D networks under aqueous conditions. The thermodynamic balance of enthalpic (ΔH) and entropic (ΔS) contributions governs network formation and material properties, allowing hydrogel behavior to be tuned through crosslinker design. Acridine-based DISHs exhibit entropy-driven binding that produces thermal stiffening. Psoralen-based DISHs exhibit dynamic behavior including shear thinning and self healing. The balance of enthalpic and entropic contributions determines binding affinity and, in turn, network structure and mechanical response. By selecting intercalators with distinct thermodynamic signatures, gelation behavior can be tuned, enabling control over the thermal and mechanical properties of the resulting hydrogel. Through cell cultures and rheology we explore how these structures effect the tunability of the hydrogels.

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