@article{TEXTUAL, recid = {13439}, author = {Neitzel, Angelika E. and Fang, Yan N. and Yu, Boyuan and Rumyantsev, Artem M. and de Pablo, Juan J. and Tirrell, Matthew V.}, title = {Polyelectrolyte Complex Coacervation across a Broad Range of Charge Densities}, journal = {Macromolecules}, address = {2021-07-06}, number = {TEXTUAL}, abstract = {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<sub>P,c</sub>) of w<sub>P,c</sub> ∼ f<sup>0.37±0.01</sup> was extracted; this trend was in good agreement with accompanying simulation predictions. Below f = 0.50, w<sub>P,c</sub> 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.}, url = {http://knowledge.uchicago.edu/record/13439}, }