PNNL

Abstract

The need for renewably sourced polymers has intensified with the worsening of global challenges such as emissions and plastic pollution. Here, we report a CO2-based poly(cyclohexene carbonate) (PCHC) vitrimer cured with zinc stearate that directly addresses both issues. Enhanced zinc dispersion within the network enabled faster curing and reprocessing than possible with zinc acetate systems, while maintaining consistent Tg and mechanical integrity across multiple cycles. The vitrimer undergoes rapid glycolysis in ethylene glycol, valorisation into ethylene carbonate with up to 97% yield without additional catalyst. When applied to carbon fibre-reinforced polymers (CFRPs), applying this strategy enabled the development of sustainable CO2-based CFRP that can undergo full resin valorisation and recovery of clean, damage-free fibres. Collectively, this tandem CO2 valorisation strategy—from vitrimer synthesis to fibre-reinforced composites and subsequent chemical upcycling—establishes multiple closed-loop recycling pathways and provides a promising route for carbon capture and utilization as well as material recycling.