Synthesis, Thermal and Mechanical Properties of Nonisocyanate Thermoplastic Polyhydroxyurethane Nanocomposites with Cellulose Nanocrystals and Chitin Nanocrystals

Wijeratne, Pavithra; Ocando, Connie; Grignard, Bruno; Berglund, Lars A.; Raquez, Jean-Marie; Zhou, Qi

doi:10.1021/acs.biomac.5c00113

Article (Scientific journals)

Synthesis, Thermal and Mechanical Properties of Nonisocyanate Thermoplastic Polyhydroxyurethane Nanocomposites with Cellulose Nanocrystals and Chitin Nanocrystals

Wijeratne, Pavithra; Ocando, Connie; Grignard, Bruno et al.

2025 • In Biomacromolecules, 26 (6), p. 3481 - 3494

Peer Reviewed verified by ORBi

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https://hdl.handle.net/20.500.12907/54144

DOI
10.1021/acs.biomac.5c00113

PubMed
40343709

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Keywords :

Bio-based; Cyclocarbonate; Green-chemistry; Mechanical and thermal properties; Multifunctionals; Nanofiller; Nonisocyanate polyurethane; Polyhydroxyurethane; Polytetramethyleneoxide; Thermal and mechanical properties; Cellulose; Chitin; Nanocomposites; Nanoparticles; Polyurethanes; Spectroscopy, Fourier Transform Infrared; Tensile Strength; Bioengineering; Biomaterials; Polymers and Plastics; Materials Chemistry

Abstract :

[en] Incorporating biobased nanofillers including cellulose nanocrystals (CNCs) and chitin nanocrystals (ChNCs) into nonisocyanate polyurethane (NIPU) offers a multifunctional approach to improving mechanical and thermal properties while promoting sustainability and green chemistry. Nanocomposites of segmented thermoplastic polyhydroxyurethane (PHU) from vanillyl alcohol bis(cyclocarbonate) (VABC), poly(tetramethylene oxide) diamine (PTMODA), and bis(aminomethyl) norbornane (NORB) reinforced with a low amount of CNCs and partially deacetylated ChNCs were prepared and characterized. Fourier transform infrared spectroscopy, atomic force microscopy, and small-angle X-ray scattering revealed that partially deacetylated ChNCs were covalently grafted to the PHU through aminolysis of carbonate end groups in the hard segment, while CNCs were mixed with the PHU without interfacial covalent bonding. Consequently, the PHU/ChNC nanocomposites showed nanophase separation with smaller hard domains compared to neat PHU, while the PHU/CNC nanocomposites exhibited a phase-mixed system with broader interface regions. Dynamic mechanical analysis and tensile tests further revealed that the PHU/ChNC nanocomposites demonstrated a 49-fold increase in Young’s modulus, a 20-fold increase in ultimate tensile strength, and a three-order-of-magnitude enhancement in storage modulus in the rubbery state compared to the PHU/CNC nanocomposites, highlighting the profound influence of interfacial covalent linkages in enhancing the thermal mechanical performance of segmented PHU.

Research center :

CIRMAP - Centre d'Innovation et de Recherche en Matériaux Polymères

Disciplines :

Materials science & engineering

Author, co-author :

Wijeratne, Pavithra ; Université de Mons - UMONS > Faculté des Sciences > Service des Matériaux Polymères et Composites ; Division of Glycoscience, Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, AlbaNova University Centre, Stockholm, Sweden

Ocando, Connie ; Laboratory of Polymeric and Composite Materials, Department of Chemistry, Faculty of Science, University of Mons, Mons, Belgium

Grignard, Bruno ; Center for Education and Research on Macromolecules (CERM), Federation of Researchers in Innovative Technologies for CO2 Transformation (FRITCO2T Research Platform), CESAM Research Unit, University of Liege, Liege, Belgium

Berglund, Lars A. ; Department of Fiber and Polymer Technology, KTH Royal Institute of Technology, Stockholm, Sweden

Raquez, Jean-Marie ; Université de Mons - UMONS > Faculté des Sciences > Service des Matériaux Polymères et Composites

Zhou, Qi ; Division of Glycoscience, Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, AlbaNova University Centre, Stockholm, Sweden

Language :

English

Title :

Synthesis, Thermal and Mechanical Properties of Nonisocyanate Thermoplastic Polyhydroxyurethane Nanocomposites with Cellulose Nanocrystals and Chitin Nanocrystals

Publication date :

09 June 2025

Journal title :

Biomacromolecules

ISSN :

1525-7797

eISSN :

1526-4602

Publisher :

American Chemical Society

Volume :

Issue :

Pages :

3481 - 3494

Peer reviewed :

Peer Reviewed verified by ORBi

Additional URL :

https://pubs.acs.org/doi/pdf/10.1021/acs.biomac.5c00113

Research unit :

S816 - Matériaux Polymères et Composites

Research institute :

R400 - Institut de Recherche en Science et Ingénierie des Matériaux

Funders :

H2020 Marie Sklodowska-Curie Actions

Funding text :

This project has received funding from the European Union\u2019s Horizon 2020 research and innovation program under the Marie Sk\u0142odowska-Curie grant agreement no. 955700. J.M.R is a FRS-FNRS Research Director and a WEL-T principal investigator from the WEL-T platform.

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