Compression-moulded and multifunctional cellulose network materials

Cellulose-based materials are widely used in a number of important applications (e.g. paper, wood, textiles). Additional developments are suggested by the growing interest for natural fibre-based composite and nanocomposite materials. The motivation is not only in the economic and ecological benefits, but is also related to advantageous properties and characteristics. The objective of this thesis is to provide a better understanding of process-structure-property relationships in some novel cellulose network materials with advanced functionalities, and showing potential large-scale processability. An important result is the favourable combination of mechanical properties observed for network-based cellulose materials. Compression-moulding of cellulose pulp fibres under high pressure (45 MPa) and elevated temperature (120 – 180 C) provides an environmentally friendly process for preparation of stiff and strong cellulose composite plates. The structure of these materials is characterized at multiple scales (molecular, supra-molecular and microscale). These observations are related to measured reduction in water retention ability and improvement in mechanical properties. In a second part, cellulose nanofibrils (NFC) are functionalized with in-situ precipitated magnetic nanoparticles and formed into dense nanocomposite materials with high inorganic content. The precipitation conditions influence particle size distributions, which in turn affect the magnetic properties of the material. Besides, the decorated NFC network provides high stiffness, strength and toughness to materials with very high nanoparticle loading (up to 50 vol.%). Subsequently, a method for impregnation of wet NFC network templates with a thermosetting epoxy resin is developed, enabling the preparation of well-dispersed epoxy-NFC nanocomposites with high ductility and moisture durable mechanical properties. Furthermore, cellulose fibrils interact positively with the epoxy during curing (covalent bond formation and accelerated curing). Potential large scale development of epoxy-NFC and magnetic nanocomposites is further demonstrated with the manufacturing of 3D shaped compression-moulded objects. Finally, the wet impregnation route developed for epoxy is adapted to prepare UVcurable NFC nanocomposite films with a hyperbranched polymer matrix. Different chemical modifications are applied to the NFC in order to obtain moisture durable oxygen barrier properties.