Liquid-Phase Condensation via Macromolecular Crowding in Polymerization-Induced Electrostatic Self-Assembly

Area of Science:

• Materials Science
• Polymer Chemistry
• Biomimetic Materials

Background:

• Macromolecular crowding is crucial for protein and membraneless organelle liquid-phase condensation.
• Its role in artificial liquid materials remains largely unexplored.

Purpose of the Study:

• To develop a strategy for creating multiphase liquid condensates with distinct charged/neutral subdomains in artificial systems.
• To explore the impact of macromolecular crowding on liquid-phase condensation in polymer self-assembly.

Main Methods:

• Utilizing reversible addition fragmentation chain transfer (RAFT) aqueous dispersion photo-copolymerization.
• Incorporating charged and neutral monomers with a polar macrochain transfer agent (CTA) and an oppositely charged polyion.
• Applying liquid-liquid phase-separation-driven polymerization-induced electrostatic self-assembly (LLPS-PIESA) with macromolecular crowding.

Main Results:

• Demonstrated self-sorting and macromolecular crowding effects during polymerization.
• Achieved the formation of nanostructured multiphase condensates with individual charged/neutral subdomains.
• Successfully adapted LLPS-PIESA to create complex artificial liquid materials.

Conclusions:

• Macromolecular crowding is a viable strategy to engineer artificial multiphase liquid condensates.
• The developed method provides access to biomimetic nanostructured materials with tunable subdomains.
• This work expands the toolkit for creating advanced functional liquid materials.