Two Synthetic Replicators Compete To Process a Dynamic Reagent Pool.

Area of Science:

• Supramolecular Chemistry
• Chemical Synthesis
• Origins of Life Research

Background:

• Dynamic covalent libraries (DCLs) offer a versatile platform for creating complex molecular systems.
• Self-replication is a fundamental process in living organisms and a key target in synthetic chemistry.

Purpose of the Study:

• To investigate the formation and behavior of self-replicating molecules within a DCL.
• To explore autocatalytic and cross-catalytic pathways in molecular self-synthesis.
• To establish the governing principles of competing replicator systems coupled to DCL processing.

Main Methods:

• Formation of a DCL from aromatic aldehydes and nucleophiles.
• Irreversible 1,3-dipolar cycloaddition reactions to form cycloadducts.
• Quantitative 19F{1H} NMR spectroscopy to monitor self-replication.
• Computational simulations to analyze kinetic and thermodynamic parameters.

Main Results:

• Two self-replicating cycloadducts (T^p and T^m) were identified within the DCL.
• These replicators utilize the DCL as feedstock for their own autocatalytic and cross-catalytic synthesis.
• Demonstrated the ability of replicators to direct their formation based on template input.
• Established relationships between kinetic/thermodynamic parameters, concentrations, and replicator competition.

Conclusions:

• Self-replicating molecules can be synthesized and controlled within a DCL environment.
• The study provides insights into the fundamental rules governing competing self-replicating systems.
• This work contributes to understanding the principles of molecular self-organization and primitive life-like behaviors.