Cellulose nanofibrils (CNFs) have been used as reinforcing elements in optically transparent composites by combination with polymer matrices. In this study, strong, optically transparent, and thick CNF/epoxy composites were prepared by immersing two or four layers of CNF sheets in epoxy resin. The morphology of the CNF, the preparation conditions of the CNF sheet, and the grammage and layer numbers of the CNF sheets were controlled. The solvent-exchanged CNF sheets resulted in the production of a composite with high transparency and low haze. The CNF with smaller width and less aggregated fibrils, which are achieved by carboxymethylation, and a high number of grinding passes are beneficial in the production of optically transparent CNF/epoxy composites. Both the grammage and number of stacked layers of sheets in a composite affected the optical and mechanical properties of the composite. A composite with a thickness of 450–800 μm was prepared by stacking two or four layers of CNF sheets in epoxy resin. As the number of stacked sheets increased, light transmittance was reduced and the haze increased. The CNF/epoxy composites with two layers of low grammage (20 g/m2) sheets exhibited high light transmittance (>90%) and low haze (<5%). In addition, the composites with the low grammage sheet had higher tensile strength and elastic modulus compared with neat epoxy and those with high grammage sheets.

Porous cellulose nanofibril (CNF) foam was prepared by stabilizing bubbles with CNF and a surfactant and then drying the stabilized wet foam in a convection oven. The consistency of carboxymethylated CNF (CMCNF) and the addition amount of the surfactant were controlled and the effects of these factors on the CNF wet foam and dry foam properties were investigated. An adequate amount of the surfactant (0.02–0.04 wt%) with CMCNF consistency higher than 0.5 wt% yielded wet foams with excellent stability. When the wet foam was dried at 60 °C in an oven, dry CNF foam with over 97% porosity was generated. The stable wet foams resulted in dry CNF foam with a sphere-like pore structure and low levels of shrinkage during drying. In contrast, unstable wet foams generated dry foam with severe shrinkage and large cavities. The pore size and the porosity of the dried foam were determined by the shape of bubbles in the wet foam and the degree of shrinkage during drying, which, in turn, affected the mechanical strength. In addition, the compressive strength of the oven-dried foam was 83% higher than that of the freeze-dried foam. Therefore, the preparation of a stable wet porous CMCNF foam by controlling the CMCNF consistency and the amount of surfactant was essential for obtaining a porous CMCNF foam with a uniform pore structure and good mechanical strength by oven drying. Graphic abstract

Cellulose nanofibril (CNF)-added polyvinylpyrrolidone (PVP) hydrogels were prepared using different types of CNFs and their properties were investigated. CNFs with different morphology and surface charge properties were prepared through quaternization and carboxymethylation pretreatments. The quaternized CNF exhibited the narrow and uniform width, and higher viscoelastic property compared to untreated and carboxymethylated CNF. When CNF was incorporated to PVP hydrogel, gel contents of all hydrogels were similar, irrespective of CNF addition quantity or CNF type. However, the absorptivity of the hydrogels in a swelling medium increased by adding CNF. In particular, the quaternized CNF-added PVP hydrogel exhibited the highest swelling ability. Unlike that of hydrogels with untreated and carboxymethylated CNFs, the storage modulus of PVP hydrogels after swelling significantly increased with an increase in the content of the quaternized CNF. These indicate that a PVP hydrogel with a high absorptivity and storage modulus can be prepared by incorporating the proper type of CNF.

Recently, enhancing the performance of polyurethane (PU) coatings with cellulose nanomaterials (CNM) has been actively researched. Cellulose nanomaterials exhibit considerable potential to increase the mechanical strength of PU coatings due to their high aspect ratios and elastic moduli. In this study, PU reinforced with CNM was coated onto paper to enhance the paper’s mechanical strength and soiling resistance. To investigate the reinforcing effect, two different CNM, cellulose nanocrystals (CNC) and 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized cellulose nanofibers (TOCN), were selected, and suspensions with different ratios of PU and CNM were prepared. After coating the paper with each of them, the mechanical properties of the paper, including tensile strength, folding endurance, and soiling resistance, were evaluated. The mechanical strength and anti-soiling performance of the PU-CNM coated papers were greatly enhanced. Especially, PU-TOCN had superior properties as a durable paper coating despite a low TOCN concentration, less than 2%, because the TOCN crosslinked with PU via polyaziridine. Furthermore, the PU-CNM coating protected the paper from being contaminated, which was confirmed by scanning electron microscopy and energy dispersive X-ray mapping. Consequently, durable paper exhibiting soiling resistance was fabricated by coating the paper with PU-TOCN suspensions.

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