[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 :
CESAM - Complex and Entangled Systems from Atoms to Materials - ULiège [BE] CERM - Center for Education and Research on Macromolecules - ULiège [BE]
Disciplines :
Materials science & engineering Chemistry
Author, co-author :
Seychal, Guillem ; University of Mons [UMons] - Center of Innovation and Research in Materials and Polymers [CIRMAP] - Laboratory of Polymeric and Composite Materials - Belgium ; University of the Basque Country - POLYMAT, Donostia/SanSebastian - Spain
Ocando, Connie ; University of Liège [ULiège] - GIGA - Department of Aerospace and Mechanical Engineering - Mechanics of Biological and Bioinspired Materials Laboratory - Belgium
Bonnaud, Leila; Materia Nova - Mons - Belgium
De Winter, Julien ; University of Mons [UMons] - Organic Synthesis and Mass Spectrometry Laboratory - Belgium
Grignard, Bruno ; University of Liège [ULiège] - Complex and Entangled Systems from Atoms to Materials [CESAM] - Research Unit, Center for Education and Research on Macromolecules [CERM] - Belgium
Detrembleur, Christophe ; University of Liège [ULiège] - Complex and Entangled Systems from Atoms to Materials [CESAM] - Research Unit, Center for Education and Research on Macromolecules [CERM] - Belgium
Sardon, Haritz ; University of the Basque Country - POLYMAT, Donostia/SanSebastian - Spain
Aramburu, Nora; University of the Basque Country - POLYMAT, Donostia/SanSebastian - Spain
Raquez, Jean-Marie ; University of Mons [UMons] - Center of Innovation and Research in Materials and Polymers [CIRMAP] - Laboratory of Polymeric and Composite Materials - Belgium
Language :
English
Title :
Emerging polyhydroxyurethanes as sustainable thermosets: a structure–property relationship
Publication date :
14 July 2023
Journal title :
ACS Applied Polymer Materials
eISSN :
2637-6105
Publisher :
American Chemical Society
Volume :
5
Issue :
7
Pages :
5567 - 5581
Peer reviewed :
Peer Reviewed verified by ORBi
Name of the research project :
The " Non-Isocyanate Polyurethanes - European Joint Doctorate " [ NIPU-EJD ]
Funders :
Marie Skłodowska-Curie Actions [BE] F.R.S.-FNRS - Fund for Scientific Research [BE] EU - European Union [BE]
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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