Poly(vinyl alcohol) (PVA) foams were prepared using a green lyophilization process without the use of foaming agents. PVA solutions with contents of CNCs (1 – 4 wt%) were prepared at two different freezing temperatures (−20 and −186 °C). With the addition of CNCs, moisture uptake of the CNC-PVA foams prepared at two freezing temperatures was lower than the neat PVA foams. With increasing CNC contents, no significant change of the moisture uptake could be observed for both types of the foams. Similar values of the moisture uptake could be found from both foams frozen at −20 and −186 °C. Scanning electron microscope measurements revealed the aligned-porous-structure of the foams frozen at −186 °C along with the ice growth direction while large and elongated pores were observed from the foams with the lower freezing temperature. These unique features of the foams prepared by a freeze-drying technique could be controlled by changing the freezing temperature, and these foams could be useful for specific applications such as tissue engineering scaffolds, thermal insulators or filters.

In this work, poly(vinyl alcohol) (PVA) and cellulose nanocrystals (CNCs) were crosslinked using sodium tetraborate decahydrate (borax) to improve the mechanical and thermal properties of the neat PVA. The results showed that the CNCs affected the crystallization behavior of the crosslinked PVA. The crystallization temperature of the crosslinked PVA with CNCs increased considerably from ∼152 to ∼187 °C. The continuous improvement of the thermal stability was observed with the increasing content of CNCs in the crosslinked PVA films. Additionally, the strong interaction between the CNCs and PVA was theoretically estimated from the Young's modulus values of the composites. Thermodynamic mechanical testing revealed that the crosslinked PVA composite films with CNCs could bear higher loads at high temperature compared to the films without the CNCs. At 60 °C, 2.7 GPa was reported for the storage modulus of the crosslinked composites with 3 wt % of CNCs, twice as high as that for the crosslinked films without CNCs. Moreover, creep results were improved when CNCs were added in the crosslinked nanocomposites. The materials prepared in this work could broaden the opportunities for applications in a wide range of temperatures.

Cellulose nanocrystal (CNC) reinforced poly(vinyl alcohol) (PVA) hydrogels with a water content of ∼92% were successfully prepared with glutaraldehyde (GA) as a cross-linker. The effects of the CNC content on the thermal stability, swelling ratio and mechanical and viscoelastic properties of the cross-linked hydrogels were investigated. The compressive strength at 60% strain for the hydrogels with 1 wt% CNCs increased by 303%, from 17.5 kPa to 53 kPa. The creep results showed that the addition of CNCs decreased the creep elasticity due to molecular chain restriction. The almost complete strain recovery (∼97%) after fixed load removal for 15 min was observed from the hydrogels with CNCs, compared with 92% strain recovery of the neat cross-linked PVA hydrogels. The incorporation of CNCs did not affect the swelling ratio and thermal stability of the hydrogels. These results suggest the cross-linked CNC-PVA hydrogels have potential for use in biomedical and tissue engineering applications.

Poly(vinyl alcohol) (PVA) foams reinforced with cellulose nanocrystals (CNCs) were prepared with formaldehyde as a crosslinking agent. Two initial reaction times (10, 120 s) and the addition of CNCs (0–2 wt% based on total reaction suspension) were found to affect the foam density, water uptake, morphology and mechanical properties. A longer initial reaction time resulted in higher mechanical properties and density, due to the small pore size. The addition of CNCs induced a progressive decrease in the pore diameter and an increase in the foam density, as well as improved mechanical properties. With 1.5 wt% CNC content, the compressive strength of the PVA foams was significantly improved from 7 to 58 kPa for 10 s-initial reaction time and from 65 to 115 kPa for 120 s-initial reaction time. Results showed that the cross-linked PVA foams with CNC had promising properties for use in biomedical applications.

This review addresses the recent developments of the processing of cellulose nanocomposites, focusing on the most used techniques, including solution casting, melt-processing of thermoplastic cellulose nanocomposites and resin impregnation of cellulose nanopapers using thermoset resins. Important techniques, such as partially dissolved cellulose nanocomposites, nanocomposite foams reinforced with nanocellulose, as well as long continuous fibers or filaments, are also addressed. It is shown how the research on cellulose nanocomposites has rapidly increased during the last 10 years, and manufacturing techniques have been developed from simple casting to these more sophisticated methods. To produce cellulose nanocomposites for commercial use, the processing of these materials must be developed from laboratory to industrially viable methods.