TY - JOUR
T1 - Chemically reactive and aging macromolecular mixtures I
T2 - Phase diagrams, spinodals, and gelation
AU - Zhang, Ruoyao
AU - Mao, Sheng
AU - Haataja, Mikko P.
N1 - Publisher Copyright:
© 2024 Author(s).
PY - 2024/6/28
Y1 - 2024/6/28
N2 - Multicomponent macromolecular mixtures often form higher-order structures, which may display non-ideal mixing and aging behaviors. In this work, we first propose a minimal model of a quaternary system that takes into account the formation of a complex via a chemical reaction involving two macromolecular species; the complex may then phase separate from the buffer and undergo a further transition into a gel-like state. We subsequently investigate how physical parameters such as molecular size, stoichiometric coefficients, equilibrium constants, and interaction parameters affect the phase behavior of the mixture and its propensity to undergo aging via gelation. In addition, we analyze the thermodynamic stability of the system and identify the spinodal regions and their overlap with gelation boundaries. The approach developed in this work can be readily generalized to study systems with an arbitrary number of components. More broadly, it provides a physically based starting point for the investigation of the kinetics of the coupled complex formation, phase separation, and gelation processes in spatially extended systems.
AB - Multicomponent macromolecular mixtures often form higher-order structures, which may display non-ideal mixing and aging behaviors. In this work, we first propose a minimal model of a quaternary system that takes into account the formation of a complex via a chemical reaction involving two macromolecular species; the complex may then phase separate from the buffer and undergo a further transition into a gel-like state. We subsequently investigate how physical parameters such as molecular size, stoichiometric coefficients, equilibrium constants, and interaction parameters affect the phase behavior of the mixture and its propensity to undergo aging via gelation. In addition, we analyze the thermodynamic stability of the system and identify the spinodal regions and their overlap with gelation boundaries. The approach developed in this work can be readily generalized to study systems with an arbitrary number of components. More broadly, it provides a physically based starting point for the investigation of the kinetics of the coupled complex formation, phase separation, and gelation processes in spatially extended systems.
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U2 - 10.1063/5.0196793
DO - 10.1063/5.0196793
M3 - Article
C2 - 38940287
AN - SCOPUS:85197145283
SN - 0021-9606
VL - 160
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 24
M1 - 244903
ER -