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A physicochemical orthophosphate cycle via a kinetically stable thermodynamically activated intermediate enables mild prebiotic phosphorylations
Nature Communications ( IF 14.7 ) Pub Date : 2021-09-17 , DOI: 10.1038/s41467-021-25555-x
Oliver R Maguire 1 , Iris B A Smokers 1 , Wilhelm T S Huck 1
Affiliation  

The incorporation of orthophosphate from scarce geochemical sources into the organic compounds essential for life under mild conditions is a fundamental challenge for prebiotic chemistry. Here we report a prebiotic system capable of overcoming this challenge by taking inspiration from extant life’s recycling of orthophosphate via its conversion into kinetically stable thermodynamically activated (KSTA) nucleotide triphosphates (e.g. ATP). We separate the activation of orthophosphate from its transfer to organic compounds by, crucially, first accumulating a KSTA phosphoramidate. We use cyanate to activate orthophosphate in aqueous solution under mild conditions and then react it with imidazole to accumulate the KSTA imidazole phosphate. In a paste, imidazole phosphate phosphorylates all the essential building blocks of life. Integration of this chemistry into a wet/dry cycle enables the continuous recycling of orthophosphate and the accretion of phosphorylated compounds. This system functions even at low reagent concentrations due to solutes concentrating during evaporation. Our system demonstrates a general strategy for how to maximise the usage of scarce resources based upon cycles which accumulate and then release activated intermediates.



中文翻译:


通过动力学稳定的热力学激活中间体进行的物理化学正磷酸盐循环可实现温和的益生元磷酸化



在温和条件下将来自稀缺地球化学来源的正磷酸盐掺入生命必需的有机化合物中是生命起源化学的一个基本挑战。在这里,我们报告了一种能够克服这一挑战的益生元系统,该系统通过从现存生命的正磷酸盐回收中汲取灵感,将其转化为动力学稳定的热力学激活(KSTA)核苷酸三磷酸(例如ATP)。至关重要的是,我们首先积累 KSTA 氨基磷酸酯,将正磷酸盐的活化与其向有机化合物的转移分开。我们在温和条件下用氰酸盐活化水溶液中的正磷酸盐,然后与咪唑反应生成KSTA咪唑磷酸盐。在糊剂中,咪唑磷酸盐磷酸化所有生命必需的组成部分。将这种化学物质集成到湿/干循环中可以实现正磷酸盐的连续回收和磷酸化化合物的积累。由于蒸发过程中溶质浓缩,该系统即使在低试剂浓度下也能发挥作用。我们的系统展示了如何基于累积然后释放激活中间体的循环来最大化稀缺资源的使用的一般策略。

更新日期:2021-09-17
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