Optimising Recycling Processes for Polyimine-Based Vitrimer Carbon Fibre-Reinforced Composites: A Comparative Study on Reinforcement Recovery and Material Properties

Abstract

We investigated the recycling process of carbon fibre-reinforced polyimine vitrimer composites and compared composites made from virgin and recycled fibres. The vitrimer matrix consisted of a two-component polyimine-type vitrimer system, and as reinforcing materials, we used nonwoven felt and unidirectional carbon fibre. Various diethylenetriamine (DETA) and xylene solvent ratios were examined to find the optimal dissolution conditions. The 20:80 DETA–xylene ratio provided efficient dissolution, and the elevated temperature (80 °C) significantly accelerated the process. Scaling up to larger composite structures was demonstrated. Scanning electron microscopy (SEM) confirmed effective matrix removal, with minimal residue on carbon fibre surfaces and good adhesion in recycled composites. The recycled nonwoven composite exhibited a decreased glass transition temperature due to the residual solvents in the matrix, while the UD composite showed a slight increase. Dynamic mechanical analysis on the recycled composite showed an increased storage modulus for nonwoven composites at room temperature and greater resistance to deformation at elevated temperatures for the UD composites. Interlaminar shear tests indicated slightly reduced adhesion strength in the reprocessed composites. Overall, this study demonstrates the feasibility of recycling vitrimer composites, emphasising the need for further optimisation to ensure environmental and economic sustainability while mitigating residual solvent and matrix effects.