This doctoral thesis investigates polyhydroxyurethanes (PHUs) as a more sustainable alternative to conventional fossil-based polymer matrices used in natural fiber-reinforced composites (NFCs). PHUs are derived from CO2-based cyclic carbonates and polyamines, making them safer and greener. They offer strong hydrogen bonding with cellulosic fibers, improved recyclability through reversible reactions, and enhanced mechanical performance, showing a 20-30% improvement over traditional epoxy composites.To make PHUs suitable for industrial applications, a copolymerization strategy was developed that improved their processability and enabled their use in techniques like resin transfer molding (RTM). The resulting composites also exhibited self-healing properties and allowed for efficient fiber recovery, with natural fibers retaining their mechanical integrity after recycling.A life cycle assessment (LCA) confirmed the environmental advantages of PHU-based composites, supporting their potential role in sustainable materials development. However, further research is needed to fully align with the European Union's sustainability goals.
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