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Stable Hg(II)-mediated base pairs with a phenanthroline-derived nucleobase surrogate in antiparallel-stranded DNA.
JBIC Journal of Biological Inorganic Chemistry ( IF 3 ) Pub Date : 2020-04-11 , DOI: 10.1007/s00775-020-01788-x
Biswarup Jash 1 , Jens Müller 1
Affiliation  

Abstract

Metal-mediated base pairs involving artificial nucleobases have emerged as a promising means for the site-specific functionalization of nucleic acids with metal ions. In this context, a GNA-appended (GNA: glycol nucleic acid) nucleoside analogue containing the artificial nucleobase 1H-imidazo[4,5-f][1,10]phenanthroline (P) has already been applied successfully in a variety of homo- and heteroleptic metal-mediated base pairs, mainly involving Ag(I) ions. Herein, we report a thorough investigation of the Hg(II)-binding properties of P when incorporated into antiparallel-stranded DNA duplexes. The artificial nucleobase P is able to form Hg(II)-mediated homoleptic base pairs of the type P–Hg(II)–P with a [2 + 2] coordination environment. In addition, the heteroleptic P–Hg(II)–T pair was investigated. The addition of a stoichiometric amount of Hg(II) to a duplex comprising either a P:P pair or a P:T pair stabilizes the DNA duplex by 4.3 °C and 14.5 °C, respectively. The P–Hg(II)–T base pair, hence, represents the most stabilizing non-organometallic Hg(II)-mediated base pair reported to date. The formation of the Hg(II)-mediated base pairs was investigated by means of temperature-dependent UV spectroscopy and CD spectroscopy.

Graphic abstract



中文翻译:

稳定的Hg(II)介导的碱基对与菲咯啉衍生的核碱基在反平行链DNA中具有替代作用。

摘要

涉及人工核碱基的金属介导的碱基对已经成为一种有希望的手段,用于利用金属离子对核酸进行位点特异性功能化。在这种情况下,包含人工核碱基1 H-咪唑并[4,5- f ] [1,10]菲咯啉(P)的添加GNA的(GNA:乙二醇核酸)核苷类似物已成功应用于多种均和杂金属介导的碱基对,主要涉及Ag(I)离子。在本文中,我们报道了掺入反平行链DNA双链体时对P的Hg(II)结合特性的彻底研究。人工核碱基P能够形成Hg(II)介导的P型同源抗体碱基对–Hg(II)– P具有[2 + 2]协调环境。此外,还研究了杂合的P –Hg(II)– T对。向包含PP对或PT对的双链体中添加化学计量的Hg(II)可使DNA双链体分别稳定在4.3°C和14.5°C的温度下。因此,P –Hg(II)– T碱基对代表了迄今为止报道的最稳定的非有机金属Hg(II)介导的碱基对。Hg(II)介导的碱基对的形成通过依赖于温度的紫外光谱和CD光谱进行了研究。

图形摘要

更新日期:2020-04-11
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