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Governed by pH‐configurable A‐motif, i‐motif and T·A‐T triplex configurations, a cascaded DNA hydrogel subjecting to diverse pH values is presented. Under highly acidic conditions (pH 1.1), N1 protonation of adenine (pKa 3.5) in A‐strands generates AH+‐H+A units, resulting in a parallel A‐motif duplex crosslinked hydrogel. Under mild acid conditions (pH 5.2), the dissociation of A‐motif duplex into...
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