In this study, pulped cellulose fibres were pre-treated with aqueous morpholine prior to mechanical disruption in the production of cellulose nanofibrils (CNF). The properties of the morpholine pretreated CNF (MCNF) were closely compared with CNF obtained from carboxymethylation (CMCNF) and TEMPO-oxidation (TCNF) pre-treatment methods. An investigation of the swelling behaviours of cellulose in varying concentrations of morpholine revealed that there is a synergistic behaviour between morpholine and water in its ability to swell cellulose. As a result, cellulose pulp dispersed in 1:1 mole ratio of morpholine to water was well swollen and readily fibrillated by mechanical shear. Surface chemistry analyses indicated that the surface of the MCNF remained unmodified, compared to the CMCNF and TCNF which were modified with anionic groups. This resulted in only a slight decrease in crystallinity index and a minimal effect on the thermal stability of MCNF, compared to CMCNF and TCNF which showed marked decreases in crystallinity indices and thermal stabilities. The average widths of MCNF, CMCNF and TCNF, as measured from electron microscopic images, were broadly similar. The higher polydispersity of MCNF widths however led to a differential sedimentation and subsequent lower aspect ratio in comparison with CMCNF and TCNF as estimated using the sedimentation approach. Also, the presence of electrostatic repulsive forces, physical interactions/ entanglements and lower rigidity threshold of the CMCNF and TCNF resulted in higher storage moduli compared to the MCNF, whose elasticity is controlled by physical interactions and entanglements. Aqueous morpholine pre-treatment can potentially be regarded as an ecologically sustainable process for unmodified CNF production, since the chemical reagent is not consumed and can be recovered and reused.

In this study, surface chemistry, the morphological properties, water retention values, linear viscoelastic properties, crystallinity index, tensile strength and thermal properties of water hyacinth (WH) cellulose were correlated with the degree of mechanical processing under high-pressure homogenisation. An initial low-pressure mechanical shear of WH stems resulted in the ease of chemical extraction of good quality cellulose using mild concentrations of chemical reagents and ambient temperature. Further passes through the homogeniser resulted in an overall improvement in cellulose fibrillation into nanofibrils, and an increase in water retention property and linear viscoelastic properties as the number of passes increased. These improvements are most significant after the first and second pass, resulting in up to 7.5% increase in crystallinity index and 50% increase in the tensile strength of films, when compared with the unprocessed WH cellulose. The thermal stability of the WH cellulose was not adversely affected but remained stable with increasing number of passes. Results suggest a high suitability for this process to generate superior quality cellulose nanofibrils at relatively low energy requirements, ideal for sustainable packaging applications and as a structural component to bioplastic composite formulations.

The effects of varying percentage loadings of morpholine pre-treated cellulose nanofibrils (MCNF) and carboxymethylated cellulose nanofibrils (CMCNF) on the aqueous swelling, compressive modulus and viscoelastic properties of calcium-ion-crosslinked alginate hydrogels were investigated. In addition, the pore structures of hydrogels with the highest compressive modulus were studied. The incorporation of 5 wt. % MCNF resulted in a slightly reduced aqueous swelling, a 36% increase in compressive modulus and a layered pore structure when compared with the neat alginate hydrogel. On the other hand, the addition of CMCNF at the same loading led to a slightly improved aqueous swelling, an increase in compressive modulus (17%) and high porosity. Further increases in CNF loadings did not result in significant increase in material properties. The alginate/CNF composite materials have potentials to be used in applications where good swelling and mechanical robustness are required.

Homogeneous high aspect ratio cellulose nanofibrils (CNFs) were prepared from Laminaria hyperborea (LH) seaweed cellulose without any initial mechanical, biological or chemical pre-treatments. Fourier-transform infrared spectrophotometry revealed that LH cellulose was of the cellulose Iα allomorph, typical of algal cellulose. Compared with wood derived CNF, significant enhancements in crystallinity, viscoelastic properties, water retention values (WRV) and morphological characteristics were identified with a single pass at 1 wt. % cellulose content through a high-pressure homogeniser. Further mechanical fibrillation did not lead to appreciable improvements in material properties that would justify the added energy consumption, which at a single pass is at least a factor of 10 lower than with wood cellulose processing. Good quality CNFs with little compromise in material properties were also obtainable at 2–3 wt. % cellulose contents as identified from viscoelastic analysis, WRV and morphological analysis. LHCNFs also showed good thermal stability, which in summary presents a multifunctional high value cellulose nanomaterial that can find application in various fields. Graphic abstract

Flexible dielectric materials with environmental-friendly, low-cost and high-energy density characteristics are in increasing demand as the world steps into the new Industrial 4.0 era. In this work, an elastomeric nanocomposite was developed by incorporating two components: cellulose nanofibrils (CNFs) and recycled alum sludge, as the reinforcement phase and to improve the dielectric properties, in a bio-elastomer matrix. CNF and alum sludge were produced by processing waste materials that would otherwise be disposed to landfills. A biodegradable elastomer polydimethylsiloxane was used as the matrix and the nanocomposites were processed by casting the materials in Petri dishes. Nanocellulose extraction and heat treatment of alum sludge were conducted and characterized using various techniques including scanning electron microscopy (SEM), thermogravimetric analysis/derivative thermogravimetric (TGA/DTG) and X-ray diffraction (XRD) analysis. When preparing the nanocomposite samples, various amount of alum sludge was added to examine their impact on the mechanical, thermal and electrical properties. Results have shown that it could be a sustainable practice of reusing such wastes in preparing flexible, lightweight and miniature dielectric materials that can be used for energy storage applications.