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构建和结构研究 DNA-联吡啶配合物作为将金属离子特异性整合到 DNA 中的通用支架。

Construction and structure studies of DNA-bipyridine complexes as versatile scaffolds for site-specific incorporation of metal ions into DNA.

机构信息

a Department of Chemistry , University at Albany, State University of New York , 1400 Washington Ave., Albany , NY 12222 , USA.

b The RNA Institute , University at Albany, State University of New York , 1400 Washington Ave., Albany , NY 12222 , USA.

出版信息

J Biomol Struct Dyn. 2019 Feb;37(3):551-561. doi: 10.1080/07391102.2018.1441071. Epub 2018 Feb 22.

Abstract

The facile construction of metal-DNA complexes using 'Click' reactions is reported here. A series of 2'-propargyl-modified DNA oligonucleotides were initially synthesized as structure scaffolds and were then modified through 'Click' reaction to incorporate a bipyridine ligand equipped with an azido group. These metal chelating ligands can be placed in the DNA context in site-specific fashion to provide versatile templates for binding various metal ions, which are exchangeable using a simple EDTA washing-and-filtration step. The constructed metal-DNA complexes were found to be thermally stable. Their structures were explored by solving a crystal structure of a propargyl-modified DNA duplex and installing the bipyridine ligands by molecular modeling and simulation. These metal-DNA complexes could have wide applications as novel organometallic catalysts, artificial ribonucleases, and potential metal delivery systems.

摘要

本文报道了一种利用“点击”反应简便构建金属-DNA 配合物的方法。首先合成了一系列 2′-炔丙基修饰的 DNA 寡核苷酸作为结构支架,然后通过“点击”反应进行修饰,引入带有叠氮基团的双吡啶配体。这些金属螯合配体可以在 DNA 中以特定的方式进行定位,为结合各种金属离子提供了多功能模板,这些金属离子可以通过简单的 EDTA 洗涤和过滤步骤进行交换。所构建的金属-DNA 配合物具有热稳定性。通过解决一个炔丙基修饰的 DNA 双链体的晶体结构,并通过分子建模和模拟安装双吡啶配体,研究了它们的结构。这些金属-DNA 配合物可作为新型有机金属催化剂、人工核酶和潜在的金属输送系统而具有广泛的应用前景。

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