Oat straw cellulose pulp was cationized in an etherification reaction with chlorocholine chloride. The cationized cellulose pulp was then mechanically disintegrated in two process steps to obtain trimethylammonium-modified nanofibrillated cellulose (TMA-NFC). The materials thus obtained were analyzed by elemental analysis, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), scanning electron microscopy (SEM) and other techniques. A higher nitrogen content of TMA-NFC samples was found by XPS analysis than by elemental analysis, which indicates that the modification occurred mainly on the surface of cellulose fibrils. XPS also confirmed the existence of ammonium groups in the samples. SEM provided images of very fine network structures of TMA-NFC, which affirmed the positive effect of ionic charge on mechanical disintegration process. According to XRD and SEM results, no severe degradation of the cellulose occurred, even at high reaction temperatures. Because of the different properties of the cationic NFC compared to negatively charged native cellulose fibers, TMA-NFC may find broad applications in technical areas, for instance in combination with anionic species, such as fillers or dyes. Indeed, TMA-NFC seems to improve the distribution of clay fillers in NFC matrix.

Recently, nanofibrillated cellulose with cationic functional groups was synthesized. This trimethylammonium-modified nanofibrillated cellulose (TMA-NFC) was applied in this study for the preparation of composites with various layered silicates. These belonged to the groups of montmorillonite, kaolin, talc, vermiculite, and mica. The respective composites were prepared by high-shear homogenization followed by filtration and hot-pressing. Data on crystal structures, chemical compositions, cation exchange capacity, specific surface area, density, and morphology of all clays and micas themselves as well as structure information of the corresponding composites have been collected. Possible microstructural features responsible for the composite appearances were tentatively identified. Principally, the interactions between TMA-NFC and the layered silicates were pronounced, due to electrostatic attraction of cationic cellulose fibrils and anionic silicate layers. This mutual interaction between TMA-NFC and layered silicate, however, was influenced not only by layered silicate properties but also by the composite preparation method, as discussed in this study.

Liquid ammonia was used to treat films of nanofibrillated cellulose (NFC), trimethylammonium-modified NFC (TMA-NFC), and their composites with vermiculite. Crystal structure, mechanical properties, water vapor permeation and water vapor adsorption of the resulting materials were investigated. Upon treatment, the crystal structure of (TMA-)NFC both in presence and absence of vermiculite changed from cellulose I to III. With the exception of TMA-NFC/vermiculite composites, pronounced effects on the addressed mechanical properties arose after exposure of the materials to ammonia. Furthermore, treatment of composite films with ammonia led to a distinct decrease in water vapor permeation. Remarkably, TMA-NFC/vermiculite composites films show the best water vapor barrier properties, high-

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