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Towards compatibilization of cellulose nanofibrils in polymer matrices

Polymer design for mediating the nanofibril–matrix interface

Time: Fri 2023-03-17 10.00

Location: F3, Lindstedtsvägen 26 & 28, Stockholm

Language: English

Subject area: Fibre and Polymer Science

Doctoral student: Rosella Telaretti Leggieri , Fiber- och polymerteknologi

Opponent: Assoc. Prof. Catarina de Carvalho Esteves, Department of Chemical Engineering and Chemistry, TU/e Eindhoven University of Technology, Netherlands

Supervisor: Professor Eva Malmström, Fiber- och polymerteknologi, Wallenberg Wood Science Center; Mats Johansson, Fiber- och polymerteknologi, Wallenberg Wood Science Center

QC 2023-02-21


Magnifying the nanostructure of wood reveals the features of an extraordinary nanocomposite material. In this nanocomposite, long fibrils of semicrystalline cellulose, with a cross-section in the nanometer range and length up to several micrometers, are embedded in an amorphous matrix made of other polymeric components. Cellulose is the load-bearing skeleton responsible for the mechanical strength of plant tissues, while the matrix cements the fibrils together and provides flexibility. 

Ever since the first methods were developed for producing individualized cellulose nanofibrils (CNFs), materials scientists have explored the potential of these biobased nanomaterials as reinforcement for nanocomposite applications. In light of the quest for renewable alternatives to fossil-based materials, both for common use and high-value applications, wood nanocomponents offer important opportunities. However, dispersing CNFs within conventional polymer matrices entails challenges related to the hydrophilic–hydrophobic character of the nanofibril–matrix interface. In this context, the aim of this thesis is to evaluate strategies for compatibilizing CNFs in relatively hydrophobic polymer matrices. 

Three different nanocomposite applications were explored by incorporating low loadings of CNFs (0.5–6 wt%) in polymer matrices. The properties of the nanofibril–matrix interface were modified by two alternative approaches, both based on the adsorption of copolymers onto CNFs in water dispersion. In the first part of the work, a tailor-made random copolymer was adsorbed onto the CNF surface and used as a macroinitiator for the in situ polymerization of methacrylate monomers by aqueous atom transfer radical polymerization (ATRP). The second part focuses on the adsorption onto CNFs of amphiphilic block copolymers synthesized by ATRP to function as CNF–matrix compatibilizers. Synthetic and analytical aspects related to the design of well-defined structures were investigated, as well as fundamental parameters affecting their adsorption onto cellulose. The use of amphiphilic block copolymers as CNF–matrix compatibilizers was explored both while targeting the dispersion of CNFs in a thermosetting coating resin, and in a thermoplastic polymer matrix. 

The outcomes of this work highlight significant effects induced by surface-modified CNFs on the structural and mechanical properties of the studied nanocomposite materials.