Dirscherl Christina F, Ianeselli Alan, Tetiker Damla, Matreux Thomas, Queener Robbin M, Mast Christof B, Braun Dieter
Systems Biophysics and Center for NanoScience, Ludwig-Maximilians-Universität München, 80799 Munich, Germany.
Phys Chem Chem Phys. 2023 Jan 27;25(4):3375-3386. doi: 10.1039/d2cp04538a.
Life is based on informational polymers such as DNA or RNA. For their polymerization, high concentrations of complex monomer building blocks are required. Therefore, the dilution by diffusion poses a major problem before early life could establish a non-equilibrium of compartmentalization. Here, we explored a natural non-equilibrium habitat to polymerize RNA and DNA. A heat flux across thin rock cracks is shown to accumulate and maintain nucleotides. This boosts the polymerization to RNA and DNA inside the crack. Moreover, the polymers remain localized, aiding both the creation of longer polymers and fostering downstream evolutionary steps. In a closed system, we found single nucleotides concentrate 10-fold at the bottom of the crack compared to the top after 24 hours. We detected enhanced polymerization for 2 different activation chemistries: aminoimidazole-activated DNA nucleotides and 2',3'-cyclic RNA nucleotides. The copolymerization of 2',3'-cGMP and 2',3'-cCMP in the thermal pore showed an increased heterogeneity in sequence composition compared to isothermal drying. Finite element models unravelled the combined polymerization and accumulation kinetics and indicated that the escape of the nucleotides from such a crack is negligible over a time span of years. The thermal non-equilibrium habitat establishes a cell-like compartment that actively accumulates nucleotides for polymerization and traps the resulting oligomers. We argue that the setting creates a pre-cellular non-equilibrium steady state for the first steps of molecular evolution.
生命基于诸如DNA或RNA等信息聚合物。对于它们的聚合作用,需要高浓度的复杂单体构建模块。因此,在早期生命能够建立非平衡的区室化之前,扩散造成的稀释是一个主要问题。在这里,我们探索了一个自然的非平衡栖息地来聚合RNA和DNA。穿过薄岩石裂缝的热通量被证明可以积累和维持核苷酸。这促进了裂缝内RNA和DNA的聚合。此外,聚合物保持在局部,有助于形成更长的聚合物并促进下游的进化步骤。在一个封闭系统中,我们发现24小时后,与裂缝顶部相比,单核苷酸在裂缝底部浓缩了10倍。我们检测到两种不同活化化学方法的聚合增强:氨基咪唑活化的DNA核苷酸和2',3'-环化RNA核苷酸。与等温干燥相比,热孔中2',3'-cGMP和2',3'-cCMP的共聚显示出序列组成的异质性增加。有限元模型揭示了聚合和积累的联合动力学,并表明在数年的时间跨度内,核苷酸从这样的裂缝中逸出的量可以忽略不计。热非平衡栖息地建立了一个类似细胞的区室,它积极积累核苷酸用于聚合,并捕获产生的寡聚物。我们认为,这种环境为分子进化的第一步创造了一个前细胞非平衡稳态。