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Bacterial nanocellulose (BNC), due to its inherent nanometric scale and strength properties, can be considered as a good candidate to be used in papermaking. This work explored the possibility of using it in the production of fine paper as a wet-end component and for the paper coating. Filler-containing handsheet production was performed with and without the presence of common additives typically used in the furnish of office papers. It was found that, under optimized conditions, BNC mechanically treated by high-pressure homogenization could improve all the evaluated paper properties (mechanical, optical and structural) without impairing the filler retention. However, paper strength was improved only to a small extent (increase in the tensile index of 8% for a filler content of ca. 27.5%). On the other hand, when used at the paper surface, remarkable improvements in the gamut area of >25% in comparison to the base paper and of >40% in comparison to only-starch coated papers were achieved for a formulation having 50% BNC and 50% of carboxymethylcellulose. Overall, the present results highlight the possibility of using BNC as a paper component, particularly when applied at the paper substrate as a coating agent aiming at improving printing quality., Fundacão para a Ciência e a Tecnologia (FCT), Portugal is acknowledged by SFRH/BDE/108095/2015 grant and Strategic Research Centre Project (UIDB/00102/2020). This work was also carried out under the Project Inpactus - innovative products and technologies from eucalyptus, Project N.º 21874 funded by Portugal 2020 through European Regional Development Fund (ERDF) in the frame of COMPETE 2020 nº246/AXIS II/2017, info:eu-repo/semantics/publishedVersion

Micro/nanofibrillated celluloses (M/NFCs) have attracted considerable research interest over the past few decades, with various pretreatments being used to reduce energy consumption and/or increase fibrillation. To date, few studies have considered cationization as a pretreatment for their preparation. In this work, quaternary ammonium groups were attached to cellulose fibers by a direct reaction with 2,3-epoxypropyltrimethylammonium chloride or by a two-step method (periodate oxidation + Girard's reagent T). The cationic fibers with degrees of substitution (DS) between 0.02 and 0.36, were subjected to homogenization treatment. The morphological properties, chemical composition, and rheological behavior were evaluated to assess the effect of DS and the effect of the cationization method (for samples with similar DS). The two-step cationization resulted in significant degradation of the cellulose structure, leading to the formation of short fibrils and solubilization of the material, ranging from 6% to almost complete solubilization at a DS of 0.36. Direct cationization resulted in longer fibrils with an average diameter of 1 μm, and no significant cellulose degradation was observed, leading to a more cohesive gel-like material (at 1 wt%). These observations clearly show the strong influence of the cationization method on the final properties of the cationic cellulosic materials.