RNA Oligomerisation without Added Catalyst from 2′,3′-Cyclic Nucleotides by Drying at Air-Water Interfaces**

IF 3.1 Q2 CHEMISTRY, MULTIDISCIPLINARY ChemSystemsChem Pub Date : 2022-09-19 DOI:10.1002/syst.202200026
Dr. Avinash Vicholous Dass, Sreekar Wunnava, Juliette Langlais, Beatriz von der Esch, Maik Krusche, Lennard Ufer, Nico Chrisam, Romeo C. A. Dubini, Dr. Florian Gartner, Severin Angerpointner, Christina F. Dirscherl, Dr. Petra Rovó, Dr. Christof B. Mast, Dr. Judit E. Šponer, Prof. Dr. Christian Ochsenfeld, Prof. Dr. Erwin Frey, Prof. Dr. Dieter Braun
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引用次数: 8

Abstract

For the emergence of life, the abiotic synthesis of RNA from its monomers is a central step. We found that in alkaline, drying conditions in bulk and at heated air-water interfaces, 2′,3′-cyclic nucleotides oligomerised without additional catalyst, forming up to 10-mers within a day. The oligomerisation proceeded at a pH range of 7–12, at temperatures between 40–80 °C and was marginally enhanced by K+ ions. Among the canonical ribonucleotides, cGMP oligomerised most efficiently. Quantification was performed using HPLC coupled to ESI-TOF by fitting the isotope distribution to the mass spectra. Our study suggests a oligomerisation mechanism where cGMP aids the incorporation of the relatively unreactive nucleotides C, A and U. The 2′,3′-cyclic ribonucleotides are byproducts of prebiotic phosphorylation, nucleotide syntheses and RNA hydrolysis, indicating direct recycling pathways. The simple reaction condition offers a plausible entry point for RNA to the evolution of life on early Earth.

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不添加催化剂的2′,3′-环核苷酸在空气-水界面干燥的RNA低聚
对于生命的出现,RNA单体的非生物合成是一个核心步骤。我们发现,在碱性、干燥的散装条件下,以及在加热的空气-水界面下,2 ',3 ' -环核苷酸在没有额外催化剂的情况下寡聚,在一天内形成多达10米。在pH值为7-12,温度为40-80°C的条件下,低聚反应继续进行,K+离子略微增强了低聚反应。在典型核糖核苷酸中,cGMP寡聚效率最高。采用HPLC - ESI-TOF联用,将同位素分布拟合到质谱上进行定量分析。我们的研究表明了一种寡聚化机制,其中cGMP有助于相对不活跃的核苷酸C, a和u的结合。2 ',3 '环核糖核苷酸是益生元磷酸化,核苷酸合成和RNA水解的副产物,表明了直接的回收途径。简单的反应条件为RNA进入早期地球生命的进化提供了一个合理的切入点。
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