Bipyridine‐Modified DNA Three‐Way Junctions with Amide linkers: Metal‐Dependent Structure Induction and Self‐Sorting. Issue 67 (19th October 2021)

• Record Type: Journal Article
• Authors: Takezawa, Yusuke; Sakakibara, Shiori; Shionoya, Mitsuhiko
• Is Part Of: Chemistry. Volume 27:Issue 67(2021)
• Page Start: 16626
• Page End: 16633
• Publication Date: 2021-10-19
• Subjects: bioinorganic chemistry -- DNA structures -- DNA three-way junctions -- metal coordination -- switching; Chemistry -- Periodicals; 540
• DOI: 10.1002/chem.202102977
• Languages: English
• ISSNs: 0947-6539

Abstract

Abstract: DNA three‐way junction (3WJ) structures are essential building blocks for the construction of DNA nanoarchitectures. We have synthesized a bipyridine (bpy)‐modified DNA 3WJ by using a newly designed bpy‐modified nucleoside, Ubpy ‐3, in which a bpy ligand is tethered via a stable amide linker. The thermal stability of the bpy‐modified 3WJ was greatly enhanced by the formation of an interstrand Ni II (bpy)3 complex at the junction core (Δ T m =+17.7 °C). Although the stereochemistry of the modification site differs from that of the previously reported bpy‐modified nucleoside Ubpy ‐2, the degree of the Ni II ‐mediated stabilization observed with Ubpy ‐3 was comparable to that of Ubpy ‐2 . Structure induction of the 3WJs and the duplexes was carried out by the addition or removal of Ni II ions. Furthermore, Ni II ‐mediated self‐sorting of 3WJs was performed by using the bpy‐modified strands and their unmodified counterparts. Both transformations were driven by the formation of Ni II (bpy)3 complexes. The structural induction and self‐sorting of bpy‐modified 3WJs are expected to have many potential applications in the development of metal‐responsive DNA materials. Abstract : Nitrogen+nickel nexus : A bipyridine‐modified DNA three‐way junction (3WJ) structure has been synthesized from three DNA strands modified with a bipyridine (bpy) ligand via a stable amide linker. The bpy‐modified 3WJ was thermally stabilized by the formation of an interstrand Ni II (bpy)3 complex. Structure induction of the 3WJs and the duplexes was achieved by addition or removal of Ni II ions. Furthermore, Ni II ‐mediated self‐sorting of 3WJs was demonstrated by using the bpy‐modified strands and their unmodified counterparts.