Abstract
Non-equilibrium, fuel-driven reaction cycles serve as model systems of the intricate reaction networks of life. Rich and dynamic behavior is observed when reaction cycles regulate assembly processes, such as phase separation. However, it remains unclear how the interplay between multiple reaction cycles affects the success of emergent assemblies. To tackle this question, we created a library of molecules that compete for a common fuel that transiently activates products. Often, the competition for fuel implies that a competitor decreases the lifetime of these products. However, in cases where the transient competitor product can phase-separate, such a competitor can increase the survival time of one product. Moreover, in the presence of oscillatory fueling, the same mechanism reduces variations in the product concentration while the concentration variations of the competitor product are enhanced. Like a parasite, the product benefits from the protection of the host against deactivation and increases its robustness against fuel variations at the expense of the robustness of the host. Such a parasitic behavior in multiple fuel-driven reaction cycles represents a lifelike trait, paving the way for the bottom-up design of synthetic life.
Highlights
In chemically fueled systems, the propensity of molecules to form assemblies is regulated by a chemical reaction cycle
We used a chemical reaction cycle that is driven by the hydration of the condensing agent ethyl-3-(3 dimethyl-aminopropyl)carbodiimide hydrochloride (EDC) (fuel, 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide)
Solving the underlying kinetic equations of the extended model, we found that the calculated data was in good agreement with the concentrations measured by high-performance liquid chromatography (HPLC) (Fig. 2D and Electronic supplementary information (ESI) Fig. 2†)
Summary
The propensity of molecules to form assemblies is regulated by a chemical reaction cycle. Brils that spontaneously self-divide,[23] temporary hydrogels,[10,35,36,37] or oil-based emulsions of which ripening is accelerated.[2] the theory on active emulsions suggests that droplets can self-divide.[38,39] More recently, examples of assemblies were observed that exert feedback over their chemical reaction cycle.[11,27,40,41] The underlying mechanisms can result in exciting behavior like the spontaneous emergence of switches between the morphologies or the ability of molecules to persist while others decay.[9,20] All these developments in the eld are incremental steps towards the synthesis of life, and a living system essentially represents a complex nonequilibrium assembly of molecules that is regulated by chemical reaction cycles.[42,43,44] in living systems, a vast number of reaction cycles operate simultaneously and interact in intricate networks through feedback mechanisms While such systems show interesting and complex emergent properties in a close-to-equilibrium context,[45,46,47,48,49,50] the behavior of multiple reaction cycles in fuel-driven synthetic systems has been underexplored. Oil droplets showed that selection and inhibition can occur in systems competing for a common fuel.[51]
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