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Abstract

DNA-based shape-memory hydrogels revealing switchable shape recovery in the presence of two orthogonal triggers are described. In one system, a shaped DNA/acrylamide hydrogel is stabilized by duplex nucleic acids and pH-responsive cytosine-rich, i-motif, bridges. Separation of the i-motif bridges at pH7.4 transforms the hydrogel into a quasi-liquid, shapeless state, that includes the duplex bridges as permanent shape-memory elements. Subjecting the quasi-liquid state to pH5.0 or Ag+ ions recovers the hydrogel shape, due to the stabilization of the hydrogel by i-motif or C-Ag+-C bridged i-motif. The cysteamine-induced transformation of the duplex/C-Ag+-C bridged i-motif hydrogel into a quasi-liquid shapeless state results in the recovery of the shaped hydrogel in the presence of H+ or Ag+ ions as triggers. In a second system, a shaped DNA/acrylamide hydrogel is generated by DNA duplexes and bridging Pb2+ or Sr2+ ions-stabilized G-quadruplex subunits. Subjecting the shaped hydrogel to the DOTA or KP ligands eliminates the Pb2+ or Sr2+ ions from the respective hydrogels, leading to shapeless, memory-containing, quasi-liquid states that restore the original shapes with Pb2+ or Sr2+ ions.

Authors

Yu, Xu;  Hu, Yuwei;  Kahn, Jason S.;  Cecconello, Alessandro;  Willner, Itamar

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