Solvent-Induced Microstructure Disruption and Catalytic Activation Synergy Toward Mild and Rapid Degradation of Epoxy Thermosets

Abstract

Epoxy thermosets' superior properties enable widespread applications, yet simultaneously impose persistent environmental burdens. Current recycling approaches remain hindered by insufficient understanding of degradation mechanisms and inadequate process control, resulting in energy-intensive degradation, low efficiency, and challenging product utilization. We have achieved here mild (60 °C) and rapid (30 min) epoxy degradation via mechanochemical pretreatment and solvent-catalyst synergism. Ball milling produces micron-scale particles through size reduction, shortening mass transfer pathways to accelerate solvent penetration. Polar solvent infiltration creates molecular highways for catalyst diffusion to ester bonds. THF disrupts microstructure to reduce mass transfer resistance, while its interaction with ethylene glycol synergistically enhances nucleophilic attack capability. This system exhibits unprecedented catalytic enhancement for 9-fold hydrolysis rate increase and 5-fold alcoholysis efficiency gain, with near-theoretical solvent economy. Crucially, vicinal diol groups in degradation products are engineered into dynamic boronate bonds, enabling closed-loop material circularity. This synchronized morphology-catalysis strategy establishes a universal paradigm for energy-efficient thermoset recycling.