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Polyelectrolyte Complex Coacervation across a Broad Range of Charge Densities.

Angelika E NeitzelYan N FangBoyuan YuArtem M RumyantsevJuan J de PabloMatthew V Tirrell
Published in: Macromolecules (2021)
Polyelectrolyte complex coacervates of homologous (co)polyelectrolytes with a near-ideally random distribution of a charged and neutral ethylene oxide comonomer were synthesized. The unique platform provided by these building blocks enabled an investigation of the phase behavior across charge fractions 0.10 ≤ f ≤ 1.0. Experimental phase diagrams for f = 0.30-1.0 were obtained from thermogravimetric analysis of complex and supernatant phases and contrasted with molecular dynamics simulations and theoretical scaling laws. At intermediate to high f, a dependence of polymer weight fraction in the salt-free coacervate phase (w P,c) of w P,c ∼ f 0.37±0.01 was extracted; this trend was in good agreement with accompanying simulation predictions. Below f = 0.50, w P,c was found to decrease more dramatically, qualitatively in line with theory and simulations predicting an exponent of 2/3 at f ≤ 0.25. Preferential salt partitioning to either coacervate or supernatant was found to be dictated by the chemistry of the constituent (co)polyelectrolytes.
Keyphrases
  • molecular dynamics simulations
  • cell free
  • body mass index
  • molecular docking
  • molecular dynamics
  • weight gain
  • single cell
  • body weight