In order to explore the reinforcing capabilities of cellulose nanofibrils, composites containing high contents of cellulose nanofibrils were prepared through a combination of water-assisted mixing and compression moulding, the components being a cellulose nanofibril suspension and an aqueous dispersion of the polyolefin copolymer poly(ethylene-co-acrylic acid). The composite samples had dry cellulose nanofibril contents from 10 to 70 vol%. Computed tomography revealed well dispersed cellulose fibril/fibres in the polymer matrix. The highest content of 70 vol% cellulose nanofibrils increased the strength and stiffness of the composites by factors of 3.5 and 21, respectively, while maintaining an elongation at break of about 5%. The strength and strain-at-break of cellulose nanofibril composites were superior to the pulp composites at cellulose contents greater than 20 vol%. The stiffness of the composites reinforced with cellulose nanofibrils was not higher than for that of composites reinforced with cellulose pulp fibres.

The mechanical and thermal properties of injection-molded recycled polyethylene were studied, specifically with respect to the influence of large-scale washing and melt-compounding of polyethylene from post-consumer packaging waste. Three types of materials were studied: those taken after sorting, after sorting and washing, and after sorting, washing, and melt-compounding, including melt-filtration, all from a large-scale material flow. The materials were further processed on a laboratory scale and compared. The results showed that large-scale washing significantly reduced thermo-oxidative stability, as well as molar mass and melt viscosity. The degradation during large-scale washing made the material susceptible to further degradation in the subsequent extrusion compounding, as shown by the differences in compounding at 240 and 200 °C using a high-shear screw configuration. The compounding parameters, screw configuration, and compounding temperature did not influence the stiffness and strength of the unwashed and large-scale-washed materials, but the elongation-at-break varied, specifically, with the increased temperature. Washing had an influence on the mechanical properties as well, and the unwashed material provided molded samples with stiffness measurements of approximately 550 MPa, whereas the large-scale-washed material provided stiffness of approximately 400 MPa. The strength measurements were approximately 15 MPa for samples made of both unwashed and large-scale-washed material, and the elongation-at-break measurements were between 50 and 150%. The large-scale-washed and compounded materials had very different mechanical properties, with stiffness measurements of approximately 320 MPa, strength of approximately 20 MPA, and elongation-at-break of approximately 350%. The significantly different mechanical properties of the large-scale-washed and compounded materials were likely due to the melt-filtration included in the compounding through the removal of metal and rubber particles, and they may also have been due to the compatibilizing and stabilizing additive used in the compounding.

Many polymers, including polyethylene, feature a relatively low melting point and hence must be cross-linked to make them viable for applications that demand a high stiffness and creep resistance at elevated temperatures. The resulting thermoset plastics cannot be recycled, and therefore alternative materials with a reconfigurable internal network structure are in high demand. Here, we establish that such a thermoset-like yet recyclable material can be realized through the addition of a nanocellulose reinforcing agent. A network consisting of cellulose nanocrystals, nano- or microfibrils imparts many of the characteristics that are usually achieved through chemical cross-linking. For instance, the addition of only 7.5 wt % of either nanocellulose material significantly enhances the melt stiffness of an otherwise molten ethylene-acrylate copolymer by at least 1 order of magnitude. At the same time, the nanocellulose network reduces the melt creep elongation to less than 10%, whereas the neat molten matrix would rupture. At high shear rates, however, the molten composites do not display a significantly higher viscosity than the copolymer matrix, and therefore retain the processability of a thermoplastic material. Repeated re-extrusion at 140 °C does not compromise the thermomechanical properties, which indicates a high degree of recyclability. The versatility of dynamic nanocellulose networks is illustrated by 3D printing of a cellulose composite, where the high melt stiffness improves the printability of the resin.

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Composites in 25 kg batches were compounded of cellulose nanocrystals (CNC) and thermomechanical pulp (TMP) and shaped into caps at industrial facilities on a pilot-plant scale. Some of the material was also injection molded into plaques to compare the effect of laboratory-scale and pilot-scale compounding of poly(ethylene-co-acrylic acid) (EAA7) and poly(caprolactone) composites reinforced with 10 wt% CNC and TMP. The materials compounded under laboratory-scale conditions showed a different morphology, improved mechanical properties, and a higher viscosity, than the materials compounded on a pilot-scale.

Hydroxyazetidinium salts were used to surface-modify cellulose nanocrystals (CNC) by grafting the salts onto the sulphate ester groups on the CNC surfaces. The grafting was confirmed by f-potential measurements and by the thermal degradation behaviour of the modified CNC. The thermal stability (onset of degradation) of the CNC was improved by the surface modification (almost 100°C). Composites containing surface-modified or unmodified CNC (0.1, 1.0 and 10 wt%) with an ethylene-based copolymer as matrix were produced by compression moulding. The thermal stability of the composites was not, however, markedly improved by the surface grafting onto the CNC. It is suggested that this is due to a degrafting mechanism, associated with the alkaline character of the system, taking place at high temperatures. Model experiments indicated, however, that this did not occur at the conditions under which the composites were produced. Furthermore, in the case of a reference based on pH-neutralised polymeric system and modified CNC, an upward shift in the onset of thermal degradation of the composite was observed. The addition of the CNC to the polymer matrix had a strong influence of the mechanical performance. For example, the tensile modulus increased approximately three times for some systems when adding 10 wt% CNC. The surface grafting of the hydroxyazetidinium salts appeared mainly to affect, in a positive sense, the yield behaviour and ductility of the composites. The results of the mechanical testing are discussed in terms of interactions between the grafted units and the matrix material and between the grafted groups.

Compression molded composites were prepared through a water-assisted mixing of an aqueous suspension of poly(ethylene-co-acrylic acid), additive, and pulp fibers [thermomechanical pulp (TMP) or dissolving pulp (DP)]. The lubricating additives used were magnesium stearate (MgSt) and molybdenum disulphide (MoS 2 ). The composite materials had dry pulp contents ranging from 30 to 70 wt% and 5 wt% additive relative to the weight of the pulp. The adsorption of the additives onto the fibers was confirmed by scanning electron microscopy and energy dispersive X-ray analysis. DMA showed that MgSt and MoS 2 gave similar interphase properties for the TMP samples at all loading contents, but the combination of MgSt and MoS 2 improved the overall properties of the DP-based composites. The tensile modulus, at 70 wt% fiber content (TMP or DP), increased compared to the matrix by a factor of 6.3 and 8.1, without lubricants, and by a factor of 8 and 10.7, with lubricants, respectively. The increase in melt viscosity observed for the lubricated samples was greater for the TMP-based samples containing MoS 2 . At a lubricant content of 5 wt%, in 30 wt% TMP, the MoS 2 behaved as both a lubricant and compatibilizer.

It is known that starch can form complexes with salts from transition and non‐transition groups, but the effect of these salts on the properties of gelatinized starch systems and their potential as alternative plasticizers has been scantily reported. In this work, the effect of adding magnesium chloride or sodium chloride to gelatinized oxidized potato starch system have been investigated. Solution cast films were characterized by their equilibrium moisture content, X‐ray diffraction spectra, dynamic mechanical thermal analysis, and tensile mechanical properties. The addition of a salt reduced the crystallinity and glass transition temperature of starch. The equilibrium moisture content increased when the Mg salt was added, but the salt recrystallization reduced the equilibrium moisture content at higher contents of NaCl. The addition of magnesium chloride resulted in lowered tensile strength and increased the elongation at break, whereas sodium chloride reduced both the tensile strength and the elongation at break.