Bipyridine-Modified DNA Three-Way Junctions with Amide Linkers: Metal-Dependent Structure Induction and Self-Sorting
Bipyridine-Modified DNA Three-Way Junctions with Amide Linkers: Metal-Dependent Structure Induction and Self-Sorting
复制标题
具有酰胺接头的联吡啶修饰 DNA 三向连接：金属依赖性结构诱导和自排序
DOI：
10.1002/chem.202102977
复制
发表时间：
2021
期刊：
影响因子：
--
通讯作者：
M. Shionoya
中科院分区：
文献类型：
--
作者：
Y. Takezawa;S. Sakakibara;M. Shionoya
DNA三向连接（3 WJ）结构是构建DNA纳米结构的基本组成部分。我们通过使用新设计的bpy修饰的核苷Ubpy-3合成了bpy修饰的DNA 3 WJ，其中bpy配体通过稳定的酰胺接头连接。通过在结核处形成链间NiII（bpy）3复合物（ΔTm=+17.7 °C），bpy修饰的3 WJ的热稳定性大大增强。尽管修饰位点的立体化学与先前报道的bpy修饰的核苷Ubpy-2不同，但用Ubpy-3观察到的NiII介导的稳定程度与Ubpy-2相当。3 WJ和双链体的结构诱导通过添加或去除NiIII离子来进行。此外，通过使用bpy修饰的链及其未修饰的对应物进行NiII介导的3 WJ自分选。这两种转化都是由NiII（bpy）3配合物的形成驱动的。bpy修饰的3 WJ的结构诱导和自分选有望在金属响应性DNA材料的开发中具有许多潜在的应用。
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 NiII(bpy)3complex at the junction core (ΔTm=+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 NiII‐mediated stabilization observed with Ubpy‐3was comparable to that of Ubpy‐2. Structure induction of the 3WJs and the duplexes was carried out by the addition or removal of NiIIions. Furthermore, NiII‐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 NiII(bpy)3complexes. 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.