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    The Impact of Surface Charges of Carboxylated Cellulose Nanofibrils on the Water Motions in Hydrated Films

    Year: 2022

    Journal: Biomacromolecules, Volume 23, AUG 8, page 3104–3115

    Authors: Guccini, Valentina; Yu, Shun; Meng, Zhoujun; Kontturi, Eero; Demmel, Franz; Salazar-Alvarez, German

    Organizations: ISIS neutron facility [2016-06959]; Swedish research council [2016-06959, 2018-06378]; FinnCERES Academy of Finland Flagship programme [318891]; Academy of Finland (AoF); AlgaLEAF [322755]; Academy of Finland (AKA) [318891] Funding Source: Academy of Finland (AKA)

    Cellulose nanofibrils (CNFs) with carboxylated surface ligands are a class of materials with tunable surface functionality, good mechanical properties, and bio-/environmental friendliness. They have been used in many applications as scaffold, reinforcing, or functional materials, where the interaction between adsorbed moisture and the CNF could lead to different properties and structures and become critical to the performance of the materials. In this work, we exploited multiple experimental methods to study the water movement in hydrated films made of carboxylated CNFs prepared by TEMPO oxidation with two different surface charges of 600 and 1550 mu mol center dot g-1. A combination of quartz crystal microbalance with dissipation (QCM-D) and small-angle X-ray scattering (SAXS) shows that both the surface charge of a single fibril and the films' network structure contribute to the moisture uptake. The films with 1550 mu mol center dot g-1 surface charges take up twice the amount of moisture per unit mass, leading to the formation of nanostructures with an average radius of gyration of 2.1 nm. Via the nondestructive quasi-elastic neutron scattering (QENS), a faster motion is explained as a localized movement of water molecules inside confined spheres, and a slow diffusive motion is found with the diffusion coefficient close to bulk water at room temperature via a random jump diffusion model and regardless of the surface charge in films made from CNFs.
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