Abstract

Models of chemical evolution are central to advancing origins of life research. To design more lifelike systems, we must expand our understanding of molecular selection mechanisms. Here, we show two selection modes that produce evolving populations of self-reproducing species, formed through thiol–disulfide exchange. Competition between thiol precursors can give clear succession patterns based on steric factors, an intrinsic property. A separate, emergent selection mechanism—dynamic activating metathesis—was found when exploring competing disulfide precursors. These experiments reveal that additional species generated in the mixture open up alternative reaction pathways to form self-reproducing products. Thus, increased compositional complexity provides certain species with a unique competitive advantage at the expense of others.

Highlights

  • Our prebiotic origins and chemical evolution are at the heart of much systems chemistry research

  • Understanding how selection may arise is key to ongoing research in dynamic systems, synthetic protocells, and replicator networks.[2−4] Even so, little is known about what selection mechanisms are available to simple replicating species competing for resources

  • Self-reproducing surfactants possess their own unique abilities and selection rules, in line with the “lipid world” theory.[16,17]. Surfactants can accelerate their own formation by forming aggregates which aid in the reaction between their phaseseparated precursors, in a process termed physical autocatalysis.[18−22] Importantly, where multiple self-reproducing species are present, surfactant production can result in a global crosscatalytic effect

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Summary

■ INTRODUCTION

Our prebiotic origins and chemical evolution are at the heart of much systems chemistry research. Self-reproducing surfactants possess their own unique abilities and selection rules, in line with the “lipid world” theory.[16,17] Surfactants can accelerate their own formation by forming aggregates which aid in the reaction between their phaseseparated precursors, in a process termed physical autocatalysis.[18−22] Importantly, where multiple self-reproducing species are present, surfactant production can result in a global crosscatalytic effect Complex systems of this type can lead to illdefined scenarios where the replication effects are tied to the system as a whole, rather than individual self-serving species. We obtain increased levels of compositional complexity which vary in time and clearly observe evolving product populations, i.e., chemical succession (Scheme 1b)

■ RESULTS AND DISCUSSION
■ CONCLUSIONS
■ ACKNOWLEDGMENTS
■ REFERENCES
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