Cyclic Processability of Functional Liquid Crystalline Epoxy Networks via Dynamic Ester Bonding

ABSTRACT Lightly crosslinked liquid crystal epoxy networks (LCENs) possess stimuli responsive shape memory behavior, making them attractive materials for sensors and actuators. However, as a thermoset epoxy, there remain significant challenges in recyclability, repairability, and processability, especially relevant for typical LCENs, which are expensive and nonbiodegradable. Herein we demonstrate the repeatable, cyclic reprocessability of a catalyzed shape‐memory liquid crystal system via dynamic covalent bonding over two distinct modes of recycling, specifically as a proof‐of‐concept for the retaining of functional properties. The introduction of dynamic ester bonding to the system enables reprocessing techniques such as repair of clean fractures and reconstitution from shredded LCEN. The recycled LCEN shows retention of shape memory behavior across several cycles of reprocessing. This work demonstrates that dynamic bonding opens the door to the synthesis of recyclable functional epoxies and serves as a starting point for sustainable epoxy designs making use of bio‐derived, repairable, dynamically‐bonded systems.