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Compatibilization of poly(methyl methacrylate) and cellulose nanocrystals through co-continuous phase to enhance the thermomechanical properties
Authors:Hichem Zergane  Saïd Abdi  Qingbo Wang  Luyao Wang  Peter Uppstu  Anna Sundberg  Chunlin Xu  Xiaoju Wang
Affiliation:1. Laboratoire des Sciences et Génie des Matériaux (LSGM), Université des Sciences et de la Technologie Houari Boumediene (USTHB), Algiers, Algeria;2. Laboratoire des Sciences et Génie des Matériaux (LSGM), Université des Sciences et de la Technologie Houari Boumediene (USTHB), Algiers, Algeria

Contribution: Project administration (lead), Resources (lead), Supervision (lead), Validation (supporting);3. Laboratory of Natural Materials Technology, Åbo Akademi University, Turku, Finland

Contribution: Data curation (equal), Software (equal), Visualization (lead);4. Laboratory of Natural Materials Technology, Åbo Akademi University, Turku, Finland

Contribution: Conceptualization (lead), Data curation (equal), Formal analysis (equal), ​Investigation (supporting);5. Polymer Technology, Laboratory of Molecular Science and Engineering, Åbo Akademi University, Turku, Finland

Contribution: Data curation (supporting), Formal analysis (supporting), Visualization (lead);6. Laboratory of Natural Materials Technology, Åbo Akademi University, Turku, Finland

Abstract:The present study focuses on enhancing the thermomechanical properties of poly(methyl methacrylate) (PMMA), a transparent and biocompatible polymer known for its high strength but limited toughness. The approach involves the development of PMMA/cellulose nanocrystals (CNCs) composites. To improve the interfacial compatibility between PMMA and CNCs, a two-step process is employed. Initially, the CNCs undergo oxidation using sodium periodate, followed by the introduction of amino groups through reductive amination. The aminated CNCs are then covalently bonded to PMMA via an amidation reaction using the “grafting onto” approach. Subsequently, the grafted CNCs are incorporated into the PMMA matrix using the solvent casting method. The resulting composites are extruded into filaments. Elemental composition analysis confirms CNC modification, revealing the presence of 1.6% nitrogen. The modified CNCs exhibit a higher degradation temperature than unmodified CNCs, showing a 50°C increase. The composites' dynamic mechanical analysis (DMA) reveals a 20% improvement in storage modulus (E′) upon incorporating 1.5% of the grafted CNCs into the PMMA matrix. This enhancement is attributed to the formation of co-continuous phases in the composite structure.
Keywords:amine functionalization  cellulose nanocrystals  co-continuous phase  grafting onto  periodate oxidation  poly(methyl methacrylate)  reductive amination
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