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This study introduces a novel liquid-liquid phase separation polymerization-induced self-assembly (PISA) method. It enables the synthesis of tunable fluidic materials like coacervate droplets and nanowires for biological applications.

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Nanotechnology

Background:

  • Polymerization-induced self-assembly (PISA) is effective for synthesizing kinetically frozen core nanoparticles.
  • The application of PISA for creating biologically relevant polymeric fluidic materials remains largely unexplored.

Purpose of the Study:

  • To introduce and validate a liquid-liquid phase separation mode of PISA.
  • To demonstrate the synthesis of tunable coacervate droplets, nanowires, and vesicles using this method.

Main Methods:

  • Utilizing visible light-initiated RAFT dispersion polymerization of an anionic monomer in the presence of protonated polyethylenimine in an aqueous solution.
  • Employing complex coacervation to drive self-assembly.
  • Investigating droplet growth mechanisms through changes in growing chain degree of polymerization (DP) or electrical neutralization.

Main Results:

  • Successfully demonstrated a stage-by-stage nano-to-micron droplet growth mechanism.
  • Showcased the interconversion between liquid coacervate droplets and glassy nanowires or vesicles by altering the ethanol/water solvent composition.
  • Achieved tunable construction of coacervate structures.

Conclusions:

  • The developed liquid-liquid phase separation PISA method offers a versatile approach for synthesizing advanced polymeric fluidic materials.
  • This technique allows for precise control over the morphology (droplets, nanowires, vesicles) of the self-assembled structures.
  • The findings open new avenues for creating bespoke polymeric materials for biological applications.