Towards a zero-waste chemcycling of thermoset polymer composites: Catalyst assisted mild solvolysis for clean carbon fiber liberation and circular coating development

Thermoset materials and their reinforced composites are widely employed in the aircraft, wind energy and construction sectors. Their 3D-crosslinked network and their chemical and physical heterogeneity make them particularly difficult to be recycled. Nowadays, the management of composite scraps and end-of-life waste is still based on landfilling or incineration practices, which are clearly non-compliant with the principles of the circular economy. In this work, a catalysed solvolysis process in mild conditions (T = 180 °C, t = 1–3 h, catalyst 1–7 wt%) was applied for the chemical recycling (chemcycling) of anhydride-cured epoxy resins and their carbon fiber reinforced composites. The selection of the hydroxylated solvents followed thermodynamic considerations (Hansen solubility parameters) and green chemistry principles. The quality of the liberated fibers was studied through thermogravimetric analysis, scanning electron microscopy and single-fiber micromechanical testing, highlighting high surface purity and 100% retention of their pristine mechanical properties (Young's modulus, elongation at break and ultimate strength). The organic recyclates were characterized through gel permeation chromatography, Fourier-transform infrared spectroscopy and chemical titration, and directly reused as hydroxylated binders for the formulation and application of bicomponent polyurethane protective coatings. The resulting coatings were characterized by high chemical resistance (> 100 double rubs at methyl-ethyl ketone test), high surface scratch hardness (3H to 5H), good substrate adhesion (1.5–4 MPa), and excellent optical clarity and surface gloss. These results demonstrate the potential zero-waste reusability of all fractions derived from the chemical recycling of carbon fiber reinforced composites, in line with the principles of the circular economy.