Exploring the untargeted synthesis of prebiotically-plausible molecules

Complex systems, prebiotic chemistry, analysis of complex mixtures, bespoke data-processing.

Colón Santos, Stephanie Marie ; Cronin, Lee

University:University of Glasgow

Department:School of Chemistry

关键词: Complex systems, prebiotic chemistry, analysis of complex mixtures, bespoke data-processing.;   

Others  :  http://theses.gla.ac.uk/75152/7/2019ColonSantosPhD.pdf

来源: University of Glasgow

【 摘 要 】

One of the biggest challenges we face when studying the Origins of Life (OoL) is that in the absence of a time-machine, it is not possible to make direct observations about what actually happened on early earth. Recently, a more ‘systems’ approach has been taken on, which looks for new phenomena and is not constrained by the search of particular products. Investigations of prebiotic complex chemical networks are increasingly tailored towards the elucidation of which environmental conditions are capable of ‘tuning’ the product distribution towards a greater degree of complexity. For this reason, a series of classic Miller-Urey experiments were conducted alongside with all-deuterated Miller-Urey experiments to explore the effect a ‘heavier’ isotope in the resulting chemical space of the complex mixture. Previous work in prebiotic chemistry has demonstrated that the inclusion of mineral surfaces in complex reaction networks, can effectively steer the product distribution into a particular product. In order to address this, we carried out the Formose reaction in a mixture of water and Formamide (50:50 v/v) and investigated how different environmental inputs (such as mineral surfaces and reaction cycling) can affect the reaction, by steering it into a particular outcome. Also, inspired by the metabolomics workflows designed for metabolite discovery, we conducted UPLC-MS/MS in a Data-Dependent fashion, which allows for features to be generated in a confident manner with each one representing a product within the complex product distribution and mapping the resulting chemical space of the products. Finally, in the case of the Miller-Urey experiment, few versions have been carried out so far (i.e. besides variations within the energy source used in the experiment or the gas mixture employed). Therefore, this prompted us to investigate the effect of reaction cycling in the Miller-Urey reaction. The effect of natural processes such as atmospheric cycling, is an important but not yet addressed variable within the prebiotic broths framework. Therefore, we decided to investigate what effect could this have in the overall product distribution of the famous experiment.