Emergence of Function and Selection from Recursively Programmed Polymerisation Reactions in Mineral Environments
Emergence of Function and Selection from Recursively Programmed Polymerisation Reactions in Mineral Environments
复制标题
矿物环境中递归编程聚合反应的函数出现和选择
DOI：
10.1002/ange.201902287
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发表时间：
2019
影响因子：
--
通讯作者：
Doran D
中科院分区：
文献类型：
--
作者：
Doran D
生命系统的特点是能够维持远离平衡的化学反应网络。生命最初很可能是通过递归反应网络中平衡状态的持续破坏过程而出现的，这一过程由周期性的环境变化驱动。在这里，我们报告了使用氨基酸和乙醇酸的递归聚合反应中出现的原酶功能。通过在每个递归循环结束时将产物以9：1稀释在新鲜的起始溶液中来保持反应不平衡，并且使用新的度量（质量指数）来探索复杂的高分子量物质的发展，该度量允许探索系统的复杂性作为循环的函数。这个过程是在一系列不同的矿物环境中进行的。我们探讨的假设，通过递归循环破坏平衡施加选择压力和随后的边界条件的产品。与非递归对照相比，仅经过四个反应循环后，递归反应的产物混合物就表现出更大的催化活性，并将产物空间截短为更高分子量的物质。
Living systems are characterised by an ability to sustain chemical reaction networks far‐from‐equilibrium. It is likely that life first arose through a process of continual disruption of equilibrium states in recursive reaction networks, driven by periodic environmental changes. Herein, we report the emergence of proto‐enzymatic function from recursive polymerisation reactions using amino acids and glycolic acid. Reactions were kept out of equilibrium by diluting products 9:1 in fresh starting solution at the end of each recursive cycle, and the development of complex high molecular weight species is explored using a new metric, the Mass Index, which allows the complexity of the system to be explored as a function of cycle. This process was carried out on a range of different mineral environments. We explored the hypothesis that disrupting equilibrium via recursive cycling imposes a selection pressure and subsequent boundary conditions on products. After just four reaction cycles, product mixtures from recursive reactions exhibit greater catalytic activity and truncation of product space towards higher‐molecular‐weight species compared to non‐recursive controls.