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Traditionally, complex coacervation is regarded as a process whereby two oppositely charged polyelectrolytes self-assemble into spherical droplets. Here, we introduce the polyzwitterionic complex, “pZC”, formed by the liquid-liquid phase separation of a polyzwitterion and a polyelectrolyte, and elucidate a mechanism by which such complexes can assemble using theory and experimental evidence. This system exhibits orthogonal phase behavior-it remains intact in acidic conditions, but disassembles as the pH increases, a process governed by the acid-base equilibria of the constituent chains. We relate the observed phase behavior to physiological conditions within the gastrointestinal tract with a simulation of the gastroduodenal junction, and demonstrate using video microscopy the viability of polyzwitterionic coacervates as technologies for the pH-triggered release of cargo. Such a system is envisaged to tackle imminent problems of drug transport via the oral route and serve as a packaging solution to increase uptake efficiency.

Coacervation in polyzwitterion-polyelectrolyte systems and their potential applications for gastrointestinal drug delivery platforms