Abstract
Chemically engineered DNAs—in which global conformation can be modulated in response to specific stimuli—could be allosteric functional DNAs themselves or work as a modulator of the functional nucleic acids such as DNAzymes and aptamers. Here, we show that two terpyridines built in the DNA backbone form a stable intramolecular 1:2 complex, [M(terpy)2](2+), with divalent transition metal ions. Upon complexation, the DNA conjugates adopt a Ω-shape structure, in which two distal sequences located outside the terpyridines connect with each other to form a continuous segment with a specific structure or sequence. Such a DNA structure is globally controlled by local metal complexation events that can be rationally designed based on general coordination chemistry. This method is regarded as metal ion-directed dynamic sequence edition or DNA splicing. DNAzymes with peroxidase-like activity can thus be regulated by several transition metal ions through sequence edition techniques based on the Ω-motif.
Highlights
Engineered DNAs—in which global conformation can be modulated in response to specific stimuli—could be allosteric functional DNAs themselves or work as a modulator of the functional nucleic acids such as DNAzymes and aptamers
We have already reported the effect of metal ions on the stability of DNA structures consisting of the conjugates with one terpy
We aimed to regulate the function of DNAzyme with peroxidase-like activity[31,32] by conformational control of the terpy2–DNA conjugate
Summary
Engineered DNAs—in which global conformation can be modulated in response to specific stimuli—could be allosteric functional DNAs themselves or work as a modulator of the functional nucleic acids such as DNAzymes and aptamers. The DNA conjugates adopt a O-shape structure, in which two distal sequences located outside the terpyridines connect with each other to form a continuous segment with a specific structure or sequence Such a DNA structure is globally controlled by local metal complexation events that can be rationally designed based on general coordination chemistry. To form such an intramolecular complex, the backbone of terpy2–DNA conjugates make adopt an O-shaped conformation, where the two distal sequences outside both terpys in the sequence are directly connected with each other to form a continuous stretch of the specific structure or sequence Such global conformational control of DNA would be regarded as metal ion-directed sequence edition or reversible splicing of DNA. We perform allosteric regulation of catalytic activity of DNAzyme through metal ion-directed sequence edition of DNA
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