Das Tamal, Ghule Siddharth, Vanka Kumar
Physical and Materials Chemistry Division, CSIR-National Chemical Laboratory (CSIR-NCL), Dr. Homi Bhabha Road, Pashan, Pune 411008, India.
Academy of Scientific and Innovative Research (AcSIR), Ghaziabad 201002, India.
ACS Cent Sci. 2019 Sep 25;5(9):1532-1540. doi: 10.1021/acscentsci.9b00520. Epub 2019 Aug 7.
The seminal Urey-Miller experiments showed that molecules crucial to life such as HCN could have formed in the reducing atmosphere of the Hadean Earth and then dissolved in the oceans. Subsequent proponents of the "RNA World" hypothesis have shown aqueous HCN to be the starting point for the formation of the precursors of RNA and proteins. However, the conditions of early Earth suggest that aqueous HCN would have had to react under a significant number of constraints. Therefore, given the limiting conditions, could RNA and protein precursors still have formed from aqueous HCN? If so, what mechanistic routes would have been followed? The current computational study, with the aid of the ab initio nanoreactor (AINR), a powerful new tool in computational chemistry, addresses these crucial questions. Gratifyingly, not only do the results from the AINR approach show that aqueous HCN could indeed have been the source of RNA and protein precursors, but they also indicate that just the interaction of HCN with water would have sufficed to begin a series of reactions leading to the precursors. The current work therefore provides important missing links in the story of prebiotic chemistry and charts the road from aqueous HCN to the precursors of RNA and proteins.
开创性的尤里 - 米勒实验表明，对生命至关重要的分子，如氰化氢（HCN），可能在冥古宙地球的还原性大气中形成，然后溶解于海洋。随后，“RNA世界”假说的支持者表明，水溶液中的HCN是RNA和蛋白质前体形成的起点。然而，早期地球的条件表明，水溶液中的HCN必须在大量限制条件下发生反应。因此，在这些限制条件下，RNA和蛋白质前体还能从水溶液中的HCN形成吗？如果可以，会遵循哪些机制途径呢？当前的计算研究借助从头算纳米反应器（AINR）——计算化学中的一种强大新工具，解决了这些关键问题。令人欣慰的是，AINR方法的结果不仅表明水溶液中的HCN确实可能是RNA和蛋白质前体的来源，还表明HCN与水的相互作用就足以引发一系列导致前体形成的反应。因此，当前的工作填补了前生物化学故事中重要的缺失环节，并描绘了从水溶液中的HCN到RNA和蛋白质前体的路径。
