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Spontaneous Formation of Core-Shell Microdroplets during Conventional Coacervate Phase Separation.

Chelsea E R Edwards1,2, Hongyi Zhang1, Ginny Wang1

  • 1Materials Research Laboratory, University of California, Santa Barbara, California 93106-9010, United States.

Langmuir : the ACS Journal of Surfaces and Colloids
|March 25, 2025
PubMed
Summary
This summary is machine-generated.

We developed a simple mixing method to create stable, core-shell coacervate droplets. These protocell-like structures, formed from poly(allylamine hydrochloride) and poly(acrylic acid), offer a new route for multiphase droplet synthesis.

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Area of Science:

  • Polymer science
  • Materials science
  • Biophysics

Background:

  • Coacervate droplets are liquid-liquid phase-separated structures with potential applications in protocell research.
  • Existing methods for creating multiphase coacervate droplets often involve complex synthesis or thermodynamic control.

Purpose of the Study:

  • To report a novel, single-step method for forming stable, core-shell coacervate droplets.
  • To investigate the formation mechanism and stability of these droplets using high-throughput microscopy and machine learning.
  • To identify conditions favoring the formation of double emulsion (DE) coacervate droplets over single emulsion (SE) droplets.

Main Methods:

  • Utilized the poly(allylamine hydrochloride) (PAH) and poly(acrylic acid) (PAA) polyelectrolyte system.
  • Employed a scalable, simple mixing process with varying compositions (polyelectrolyte ratios, salt concentrations) and processing routes (mixing rate, thermodynamic path).
  • Applied high-throughput microscopy and machine learning for droplet morphology classification and analysis.

Main Results:

  • Achieved single-step formation of protocell-like, core-shell coacervate droplets with a polyelectrolyte-rich shell and solvent-rich core.
  • Observed coexistence of DE and single emulsion (SE) droplets, indicating a kinetic formation mechanism.
  • Found that DE droplets preferentially form over SE droplets at a wide range of compositions with a slow injection mixing rate, lower salt concentrations, and near 1:1 charge stoichiometry (favoring polycation excess).
  • Demonstrated stability of DE droplets to the micron scale, even after coalescence, though they are metastable and stabilized by shell viscoelasticity and viscosity.

Conclusions:

  • The developed scalable, simple mixing process provides a novel and orthogonal mechanism for producing multiphase coacervate droplets.
  • This method bypasses the need for dropwise synthesis or thermodynamic tuning required by existing routes.
  • The findings contribute to the understanding and scalable production of complex coacervate structures for potential applications.