Emergence of Function and Selection from Recursively Programmed Polymerisation Reactions in Mineral Environments.
David DoranYousef M Abul-HaijaLeroy CroninPublished in: Angewandte Chemie (International ed. in English) (2019)
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.