Abstract
The continuous consumption of chemical energy powers biological systems so that they can operate functional supramolecular structures. A goal of modern science is to understand how simple chemical mixtures may transition from non-living components to truly emergent systems and the production of new lifelike materials and machines. In this work a replicator can be maintained out-of-equilibrium by the continuous consumption of chemical energy. The system is driven by the autocatalytic formation of a metastable surfactant whose breakdown products are converted back into building blocks by a chemical fuel. The consumption of fuel allows the high-energy replicators to persist at a steady state, much like a simple metabolic cycle. Thermodynamically-driven reactions effect a unidirectional substrate flux as the system tries to regain equilibrium. The metastable replicator persists at a higher concentration than achieved even transiently in a closed system, and its concentration is responsive to the rate of fuel supply.
Highlights
The continuous consumption of chemical energy powers biological systems so that they can operate functional supramolecular structures
Macrocyclic disulfides within a dynamic combinatorial library, as developed by Otto, are formed autocatalytically via fibrous stacks, whose breakage and exposure of fibre ends leads to an increase in the macrocyclic building blocks (Fig. 1b)
Systems operating under a continuous consumption of a chemical fuel would have greater similarity to biological dissipative structures[7]
Summary
The continuous consumption of chemical energy powers biological systems so that they can operate functional supramolecular structures. Stable replicators (Fig. 1a), which are not subject to a destruction reaction, will move to equilibrium after the consumption of starting materials. Whilst kinetically trapped replicators are not at the thermodynamic minimum, they are not in an energy-consuming, dissipative, out-of-equilibrium state (Fig. 1b).
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