Synthesis of microporous hydrogen-bonded supramolecular organic frameworks through guanosine self-assembly
Synthesis of microporous hydrogen-bonded supramolecular organic frameworks through guanosine self-assembly
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DOI：
10.1016/j.xcrp.2021.100519
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发表时间：
2021-08-18
影响因子：
8.9
通讯作者：
Shi, Xiaodong
中科院分区：
文献类型：
--
作者：
He, Ying;Zhang, Yanbin;Shi, Xiaodong
通过小分子自组装扩展结构层次和复杂性是获得大型离散功能分子结构的有效方法。通过简单的鸟苷单体自组装，在固态下构建了具有纳米尺寸孔的氢键超分子有机框架（HsOF）。为了将G四联体自组装的层次结构扩展到比传统G四联体更高的级别，在鸟苷的C-8位置上引入H键受体，通过与相邻G四联体的N(2)-H-B的H键合建立四联体间连接。经过筛选不同的C-8取代基和各种合成条件后，在稀释条件下通过溶剂蒸发得到HsOF-G1a'。单晶X射线结构表明，G(8)形成的立方重复单元是具有大孔(d = 34 A)的超分子二级构件(SBU)。据我们所知，这是第一个具有超越圆柱形 G 四联体的有组织结构的 G 四联体自组装。
Extending the structural hierarchy and complexity through small-molecular self-assembly is a powerful way to obtain large discrete, functional molecular architecture. A hydrogen-bonded supramolecular organic framework (HsOF) with nanometer-size pores is constructed in a solid state with simple guanosine-monomer self-assembly. To extend the hierarchy of the G-quartet self-assembly to a higher order than that of the traditional G-quadruplex, H-bond acceptors on the C-8 position of guanosine are introduced to establish inter-quadruplex linkage via H bonding to N(2)-H-B from the neighboring G-quartet. After screening different C-8 substitution groups and various synthesis conditions, HsOF-G1a' is obtained by solvent evaporation under diluted condition. Single-crystal X-ray structure reveals that cubic repeating units formed by G(8) are the supermolecule secondary building block (SBU) with large pores (d = 34 A). To our knowledge, this is the first G-quartet self-assembly with an organized structure beyond cylindrical G-quadruplexes.