The threshold complexity required for the chemical emergence of living matter necessitates the integration of catalytic competency with self-replicating capability operating out of equilibrium. Herein, we report on a catalytic self-replicating system that demonstrates complex behavior from a short peptide building block under non-equilibrium conditions. In a closed system, two distinct populations of imine-based peptide building blocks replicate with an antagonistic relationship exclusively under a non-equilibrium regime by turning over a thermodynamically activated substrate to low-energy waste. Catalytic self-destruction of the preceding replicating entities through substrate degradation (negative feedback) allows replicating networks to adapt and select a new set of fitter successor replicators through catalysis-mediated alteration in the environment (feedforward activation). Mimicking such complex behavior under non-equilibrium conditions foreshadows the emergence of Darwinian threshold (ribosomes integrate catalysis and replication), which is required for realizing systems with living matter-like properties.

Foreign