Nucleotide Selectivity in Abiotic RNA Polymerization Reactions.
Nucleotide Selectivity in Abiotic RNA Polymerization Reactions.
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DOI：
10.1007/s11084-017-9532-7
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发表时间：
2017-09
期刊：
影响因子：
--
通讯作者：
McGown LB
中科院分区：
文献类型：
--
作者：
Coari KM;Martin RC;Jain K;McGown LB
为了在早期地球上建立一个RNA世界，核苷酸必须通过化学反应而不是生化反应形成聚合物。聚合产物必须足够长，以执行催化功能，包括自我复制，并保存遗传信息。这些功能不仅取决于聚合物的长度，还取决于它们的序列。到目前为止，对非生物RNA聚合的研究一般集中在单核苷酸的聚合路线和均聚产物的长度上。较少的工作是在反应的选择性上将一些核苷酸掺入核苷酸混合物中而不是其他核苷酸。这些信息对于理解RNA的化学进化是必不可少的一步。为了解决这个问题，在本工作中，RNA聚合反应是在蒙脱石粘土催化剂存在下进行的。核苷酸包括单磷酸腺苷、胞苷、鸟苷、尿苷和肌苷。实验包括咪唑激活的核苷酸(ImpX)与一个或多个未激活的核苷酸(XMP)的混合物、两个或更多ImpX的混合物以及在聚合反应本身中原位激活的XMP的反应。反应产物用基质辅助激光解吸电离飞行时间质谱仪(MALDI-TOF MS)分析，以确定聚合产物的长度和核苷酸组成。结果表明，不同核苷酸的聚合度、杂聚度和均聚度以及聚合产物的组成都不同，这取决于混合物中存在哪些核苷酸和多少不同的核苷酸。
In order to establish an RNA world on early Earth, the nucleotides must form polymers through chemical rather than biochemical reactions. The polymerization products must be long enough to perform catalytic functions, including self-replication, and to preserve genetic information. These functions depend not only on the length of the polymers, but also on their sequences. To date, studies of abiotic RNA polymerization generally have focused on routes to polymerization of a single nucleotide and lengths of the homopolymer products. Less work has been done the selectivity of the reaction toward incorporation of some nucleotides over others in nucleotide mixtures. Such information is an essential step toward understanding the chemical evolution of RNA. To address this question, in the present work RNA polymerization reactions were performed in the presence of montmorillonite clay catalyst. The nucleotides included the monophosphates of adenosine, cytosine, guanosine, uridine and inosine. Experiments included reactions of mixtures of an imidazole-activated nucleotide (ImpX) with one or more unactivated nucleotides (XMP), of two or more ImpX, and of XMP that were activated in situ in the polymerization reaction itself. The reaction products were analyzed using matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) to identify the lengths and nucleotide compositions of the polymerization products. The results show that the extent of polymerization, the degree of heteropolymerization vs. homopolymerization, and the composition of the polymeric products all vary among the different nucleotides and depend upon which nucleotides and how many different nucleotides are present in the mixture.
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