Anion-π interaction-induced phase separation as a prebiotic pathway to oxygenation

Area of Science:

• Prebiotic Chemistry
• Supramolecular Chemistry
• Origins of Life Research

Background:

• Prebiotic chemistry relies on compartmentalization and reactivity for evolution.
• The interplay between compartment chemistry and intrinsic activity is understudied.
• Anion-π interactions are overlooked in phase transition chemistry.

Purpose of the Study:

• To explore the coupling of compartmentalization chemistry with intrinsic chemical activity.
• To demonstrate how anion-π interactions can drive the formation of functional assemblies.
• To provide a plausible prebiotic pathway for bioenergetics and oxygen generation.

Main Methods:

• Investigating anion-π interactions in phase transition chemistry.
• Demonstrating the formation of micron-sized assemblies driven by anion-π interactions.
• Characterizing the electrochemical environments of these assemblies and their reactivity.

Main Results:

• Anion-π interactions drive the formation of micron-sized assemblies.
• These assemblies recruit cations to form anion-π-cation triads.
• Assemblies mediate spontaneous oxygenation reactions via their electrochemical environments.
• This leads to primitive pigment formation and oxidation-dependent protocell selection.

Conclusions:

• Anion-π interactions introduce chemical functions into self-assembly and phase transition.
• This provides a plausible prebiotic pathway for bioenergetics and oxygen generation on early Earth.
• Findings offer principles for engineering electrochemically active supramolecular assemblies and understanding abiotic evolution.