[en] Polyhydroxyurethanes (PHU), obtained from CO2-based cyclic carbonates (CC) and polyamines, are known as greener and safer alternatives to conventional polyurethanes. Interestingly, the hydroxyurethane moieties present along the PHU’s backbone offer unexplored opportunities in terms of enhanced adhesion and mechanical properties that could be a major breakthrough in many structural applications. Furthermore, PHUs have shown thermomechanical recyclability arising from the ability of hydroxyurethane moieties to participate in reversible exchange reactions. However, the relationship between the macromolecular structure, the processability, and the final properties of these materials have not been evaluated to a sufficient extent to establish a comprehensive overview of these emerging thermosets. In this sense, this work aims to address this research gap by investigating the rheological and thermomechanical performances of PHU thermosets and opening an unexplored door for future sustainable engineered structural applications. A special emphasis was put on PHU thermosets formulated using potentially biobased monomers. The rheological behavior during cross-linking of the PHU formulations was studied and highlighted the importance of the number of CC functionalities in the viscosity and gel time, ranging from 10 min to nearly 3 h. Moduli superior to 2 GPa and glass transition over 50 °C were obtained for short multifunctional CC. Finally, the dynamic network behavior of these PHUs was also demonstrated through stress-relaxation and reprocessing. High temperatures (over 150 °C) and pressure lead to a good recovery of the thermomechanical properties. Such materials appear to be an interesting platform for structural applications, particularly fiber-reinforced polymers, that can overcome many sustainability challenges.
Research center :
CIRMAP - Centre d'Innovation et de Recherche en Matériaux Polymères
Disciplines :
Chemistry
Author, co-author :
Seychal, Guillem ; Université de Mons - UMONS > Faculté des Science > Service des Matériaux Polymères et Composites ; POLYMAT and Department of Advanced Polymers and Materials: Physics, Chemistry, and Technology, Faculty of Chemistry, University of the Basque Country UPV/EHU, Donostia-San Sebastián, Spain
Ocando, Connie ; Laboratory of Polymeric and Composite Materials, Center of Innovation and Research in Materials and Polymers (CIRMAP), University of Mons, Mons, Belgium
Bonnaud, Leila ; Université de Mons - UMONS > Unités externe > Materia Nova ASBL ; Materia Nova asbl, Parc Initialis, Mons, Belgium
De winter, Julien ; Université de Mons - UMONS > Faculté des Science > Service de Synthèse et spectrométrie de masse organiques
Grignard, Bruno ; Department of Chemistry, Center for Education and Research on Macromolecules (CERM), University of Liége, Sart-Tilman, Liége, Belgium
Detrembleur, Christophe; Department of Chemistry, Center for Education and Research on Macromolecules (CERM), University of Liége, Sart-Tilman, Liége, Belgium
Sardon, Haritz ; POLYMAT and Department of Advanced Polymers and Materials: Physics, Chemistry, and Technology, Faculty of Chemistry, University of the Basque Country UPV/EHU, Donostia-San Sebastián, Spain
Aramburu, Nora; POLYMAT and Department of Advanced Polymers and Materials: Physics, Chemistry, and Technology, Faculty of Chemistry, University of the Basque Country UPV/EHU, Donostia-San Sebastián, Spain
Raquez, Jean-Marie ; Université de Mons - UMONS > Faculté des Science > Service des Matériaux Polymères et Composites
Language :
English
Title :
Emerging Polyhydroxyurethanes as Sustainable Thermosets: A Structure-Property Relationship
Research Institute for Materials Science and Engineering
Funders :
H2020 Marie Sklodowska-Curie Actions
Funding text :
The authors would like to express thanks for the financial support provided by the NIPU-EJD project; this project has received funding from the European Union’s Horizon 2020 research and innovation program under Marie Skłodowska-Curie Grant Agreement No. 955700. The authors are also grateful to the Materia Nova technological platform (Mons, Belgium) for the support in rheology and characterization. Christophe Detrembleur is the F.R.S.-FNRS Research Director.
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