Abstract
Development of a metal-mediated base paring system has expanded the functions of DNA-based materials. We have recently reported that a 5-hydroyxuracil (UOH) nucleobase forms both a metal-mediated self-base pair (UOH–M–UOH; M=Gd(III) etc.) and a Watson–Crick-type hydrogen-bonded base pair with adenine nucleobase (UOH–A). In this study, we have investigated the pH-dependence of the thermal stability of DNA duplexes containing UOH–M–UOH base pairs or UOH–A base pairs in the absence or presence of Gd(III) or Zn(II) ions. Melting experiments and UV absorption analyses revealed that the complexation of UOH bases with Zn(II) ions altered the thermal stability of the DNA duplexes in a pH-dependent manner. In the presence of Zn(II) ions, a UOH–UOH-containing duplex was stabilized at higher pH while a UOH–A-containing duplex was destabilized. This pH-dependence of the metallo-DNA structures containing UOH nucleobases is specific to Zn(II) ions. Such dual responsiveness to both pH and metal ions would enrich switchable functions of metallo-DNA-based materials.
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