Exploring the mean-field phase behavior of binary vitrimer networks

Vitrimers, polymer networks featuring associative dynamic bonds, have garnered significant attention for their diverse applications, including self-healing, shape memory, and reprocessibility. The incorporation of phase-separating components in vitrimers further expands the design space for these properties. This study investigates the phase behavior of vitrimers formed by crosslinking binary blends with three-armed crosslinkers. We employ self-consistent field theory to model the phase behavior of these systems, accounting for junction points in a mean-field fashion by (1) incorporating kinetic rate equations during field updates to account for bond exchange and (2) quantifying the associated combinatorial entropy for the junctions. The latter is anticipated to be a key factor influencing the phase behavior of these binary vitrimers. This research aims to provide deeper insights into the complex interplay between network dynamics and phase separation in vitrimers, potentially guiding future design strategies for advanced functional or recyclable materials.