具有连续AgI-Mediated主链的平行G-双链和C-双链DNA
Parallel G-duplex and C-duplex DNA with Uninterrupted Spines of AgI-Mediated Base Pairs
摘要：
核碱基之间的氢键产生不同的DNA结构基序，包括典型的双链体、鸟嘌呤（G）四链体和胞嘧啶（C）i-基序。将金属介导的碱基对引入核酸结构中可以引入新的功能和增强的稳定性。在这里，我们证明，使用质谱（MS），离子迁移谱（IMS）和荧光共振能量转移（FRET），由多达20个G-Ag（I）-G连续碱基对组成的平行链结构形成时，天然DNA序列与银阳离子在水溶液中混合。FRET表明由具有20个连续C-Ag（I）-C碱基对的聚（胞嘧啶）链形成的双链体也是平行的。银介导的G-双链体优先于G-四链体形成，并且Ag+将G-四链体转化为银配对双链体的能力可能提供操纵这些生物相关结构的新途径。IMS表明，G-双链体是线性的，比B-DNA更刚性。DFT计算用于提出与IMS实验兼容的结构。这种廉价、无缺陷且可溶的DNA基纳米线为新型金属介导的DNA纳米技术的设计开辟了新的方向。
英文摘要：
Hydrogen bonding between nucleobases produces diverse DNA structural motifs, including canonical duplexes, guanine (G) quadruplexes and cytosine (C) i-motifs. Incorporating metal-mediated base pairs into nucleic acid structures can introduce new functionalities and enhanced stabilities. Here we demonstrate, using mass spectrometry (MS), ion mobility spectrometry (IMS) and fluorescence resonance energy transfer (FRET), that parallel-stranded structures consisting of up to 20 G-Ag(I)-G contiguous base pairs are formed when natural DNA sequences are mixed with silver cations in aqueous solution. FRET indicates that duplexes formed by poly(cytosine) strands with 20 contiguous C-Ag(I)-C base pairs are also parallel. Silver-mediated G-duplexes form preferentially over G-quadruplexes, and the ability of Ag+ to convert G-quadruplexes into silver-paired duplexes may provide a new route to manipulating these biologically relevant structures. IMS indicates that G-duplexes are linear and more rigid than B-DNA. DFT calculations were used to propose structures compatible with the IMS experiments. Such inexpensive, defect-free and soluble DNA-based nanowires open new directions in the design of novel metal-mediated DNA nanotechnology.
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