从氰化氢水溶液中形成核糖核酸和蛋白质前体的热可及益生元途径,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

从氰化氢水溶液中形成核糖核酸和蛋白质前体的热可及益生元途径
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-03-07 , DOI: 10.1021/jacs.2c11857
Qiyuan Zhao ₁ , Sanjay S Garimella ₁ , Brett M Savoie ₁

Affiliation

寻找与生物学相关的分子的生命起源前化学途径是一个长期存在的难题，它产生了一系列相互竞争的假设，而这些假设的证伪实验前景有限。然而，计算网络探索方法的出现创造了机会来比较各种渠道的动力学合理性，甚至提出新的途径。在这里，可以在水和氰化氢 (HCN) 的四个极性或周环反应中形成的有机分子空间，这两个已确定的用于生成生物前体的生命前候选物，已通过最先进的探索算法进行了全面探索。在这些简单分子的短短几步之内，就揭示了令人惊讶的多样化反应景观。与最近提出的替代方案相比，发现了几种生物学相关分子的反应途径涉及较低的活化能和较少的反应步骤。考虑水催化反应定性地影响网络动力学的解释。该案例研究还强调了其他算法对某些产品的更简单和更低屏障的反应途径的遗漏，这些算法定性地影响了 HCN 反应性的解释。

"点击查看英文标题和摘要"

Thermally Accessible Prebiotic Pathways for Forming Ribonucleic Acid and Protein Precursors from Aqueous Hydrogen Cyanide

The search for prebiotic chemical pathways to biologically relevant molecules is a long-standing puzzle that has generated a menagerie of competing hypotheses with limited experimental prospects for falsification. However, the advent of computational network exploration methodologies has created the opportunity to compare the kinetic plausibility of various channels and even propose new pathways. Here, the space of organic molecules that can be formed within four polar or pericyclic reactions from water and hydrogen cyanide (HCN), two established prebiotic candidates for generating biological precursors, was comprehensively explored with a state-of-the-art exploration algorithm. A surprisingly diverse reactivity landscape was revealed within just a few steps of these simple molecules. Reaction pathways to several biologically relevant molecules were discovered involving lower activation energies and fewer reaction steps compared with recently proposed alternatives. Accounting for water-catalyzed reactions qualitatively affects the interpretation of the network kinetics. The case-study also highlights omissions of simpler and lower barrier reaction pathways to certain products by other algorithms that qualitatively affect the interpretation of HCN reactivity.

更新日期：2023-03-07

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南