Environmental conditions drive self-organization of reaction pathways in a prebiotic reaction network

Abstract

The evolution of life from the prebiotic environment required a gradual process of chemical evolution towards greater molecular complexity. Elaborate prebiotically-relevant synthetic routes to the building blocks of life have been established. However, it is still unclear how functional chemical systems evolved with direction using only the interaction between inherent molecular chemical reactivity and the abiotic environment. Here, we demonstrate how complex systems of chemical reactions exhibit well-de ned selforganisation in response to varying environmental conditions. This self-organisation allows the compositional complexity of the reaction products to be controlled as a function of factors such as feedstock and catalyst availability. We observe how Breslow's cycle contributes to the reaction composition by feeding C 2 building blocks into the network, alongside reaction pathways dominated by formaldehyde-driven chain growth. The emergence of organised systems of chemical reactions in response to changes in the environment offers a potential mechanism for a chemical evolution process that bridges the gap between prebiotic chemical building blocks and the origin of life.

Dynamic Environmental Conditions Affect the Composition of a Model Prebiotic Reaction Network

“…The influence of temporal fluctuations on formose reactions was studied at a fixed inlet dihydroxyacetone concentration (50 mM) and three different inlet formaldehyde concentrations (20, 50, and 100 mM). These conditions covered previously identified organizational patterns which were dominated by either aldol addition reactions of C 2 and C 3 carbohydrates ([formaldehyde] in = 20 mM) ,,, or by addition reactions of formaldehyde to sugar enolates in the network ([formaldehyde] in = 100 mM) , as well as a condition intermediate between the two ([formaldehyde] in = 50 mM) …”

“…The reactivity of the formose reaction can be rationalized using enolate, aldol addition, and Cannizzaro reactions, providing a well-defined space from which underlying reaction pathways can be inferred (Figure 1a). [23][24][25][26][27]29,30 Thus, the formose reaction is an excellent model system which provides access to a variety of reactions, compounds, and conditional sensitivities under "one pot" conditions.…”

Chemically Driven Multimodal Locomotion of Active, Flexible Sheets

“…In the human body, functionality is regulated by a chain of interlinked chemical reactions. − These chemical reaction networks (CRNs) operate in fluids that are confined between soft structural walls, such as those bounding cells and internal organs . Based on findings on synthetic materials systems, it is conceivable that these reaction networks trigger flow in the confined biological fluids.…”

Extended Curtin-Hammett principle: Origin of pathway selection in reversible reaction networks under kinetic control

“…Although kinetics of the elementary reactions in the network are very simple, unexpected results like emergence are sometimes observed due to mutual correlation among the reactions. Such emergent behaviors have been analyzed and understood by mathematical models, [29][30][31][32][33] which enable us to abstract universality in similar and related phenomena. [34][35][36] Most of above-mentioned systems are composed of irreversible reactions, so the direction of each elementary reaction is basically determined.…”