Preparation and Viscoelastic Properties of Composite Fibres Containing Cellulose Nanofibrils: Formation of a Coherent Fibrillar Network

Composite fibres with a matrix of poly(ethylene glycol) (PEG) and cellulose nanofibrils (CNF) as reinforcing elements were produced using a capillary viscometer. Two types of CNF were employed: one based on carboxymethylated pulp fibres and the other on TEMPO-oxidized pulp. Part of the latter nanofibrils was also grafted with PEG in order to improve the compatibility between the CNF and the PEG matrix. The nominal CNF-content was kept at 10 or 30 weight-%. The composite fibres were characterized by optical and scanning electron microscopy in addition to dynamic mechanical thermal analysis (DMTA). Evaluation of the storage modulus indicated a clear reinforcing effect of the CNF, more pronounced in the case of the grafted CNF and depending on the amount of CNF. An interesting feature observed during the DMTA-measurements was that the fibrils within the composite fibres appeared to forma rather coherent and load-bearing network which was evident even after removing of the PEG-phase (by melting). An analysis of the modulus of the composite fibres using a rather simple model indicated that the CNF were more efficient as reinforcing elements at lower concentrations which may be associated with a more pronounced aggregation as the volume fraction of CNF increased