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Complex coacervation, known as the liquid-liquid phase separation ofsolutions with oppositely charged polyelectrolytes, has attracted substantialinterest in recent years. We study the effect of the charge regulation (CR)mechanism on the complex coacervation by including short-range interactionsbetween the charged sites on the polymer chains as well as anassociation-dissociation energy parameter in the CR mechanism. We investigatethe phase diagrams of two CR models: (i) the hopping CR model (HCR) and (ii)the asymmetric CR model (ACR). It is shown that during the phase separationthat the polymers in the condensed phase are more charged than those in thedilute phase, in accordance with Le Chatelier's principle. In addition,secondary CR effects also influence the change in the volume fraction of thetwo phases. The latter can cause the charge difference between the two phasesto change nonmonotonically as a function of the CR parameters.

Phase Separation of Polyelectrolytes: The Effect of Charge Regulation