在机器人化学计算机系统中执行的矿物介导聚合反应中的选择证据

IF 3.1 Q2 CHEMISTRY, MULTIDISCIPLINARY ChemSystemsChem Pub Date : 2024-03-07 DOI:10.1002/syst.202400006
Silke Asche, Robert W. Pow, Hessam M. Mehr, Geoffrey J. T. Cooper, Abhishek Sharma, Prof. Leroy Cronin
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引用次数: 0

摘要

长期以来,人们一直认为生物的产生需要一个分子水平的选择和进化过程,但这一过程很难通过实验来探索。解决方案之一是在实验中使用自动化,这样可以实现可追溯性,并能探索更大的反应空间。我们报告了一个完全可编程的自动化平台,用于探索氨基酸在矿物环境中的反应。机器人系统以 Chemputer 系统为基础,该系统具有定义明确的模块、软件和化学编程语言,可协调包括分析在内的化学过程。反应混合物采用串联质谱法和肽测序算法进行分析。每次实验都筛选出 1,398,100 个可能的独特序列,并通过实验确认了超过 550 个明确定义的序列。这项工作旨在对重复聚合反应循环中的选择形成新的认识,以探索定义明确的氨基酸序列的出现。我们发现,不同矿物质的存在对低聚物的结果有显著影响,蛇纹石环境会选择富含甘氨酸和苯丙氨酸的片段,从而形成具有明确序列的较长的低聚物,这与循环次数有关。
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Evidence of Selection in Mineral Mediated Polymerization Reactions Executed in a Robotic Chemputer System

It has long been thought that abiogenesis requires a process of selection and evolution at the molecular level, but this process is hard to explore experimentally. One solution could be the use of automation in experiments which could allow for traceability and the ability to explore a larger reaction space. We report a fully programmable and automated platform to explore the reactions of amino acids in the presence of mineral environments. The robotic system is based upon the Chemputer system which has well defined modules, software, and a chemical programming language to orchestrate the chemical processes, including analysis. The reaction mixtures were analysed with tandem mass spectrometry and a peptide sequencing algorithm. Each experiment was screened for 1,398,100 possible unique sequences, and more than 550 specifically defined sequences were confirmed experimentally. This work aimed to develop a new understanding of selection in repeated cycles of polymerisation reactions to explore the emergence of well-defined amino acid sequences. We found that the outcome of oligomerisation was significantly influenced by the presence of different minerals, and that a serpentine environment selects glycine and phenylalanine rich fragments that enable the formation of longer oligomers with well-defined sequences as a function of cycle number.

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