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Edge-On (Cellulose II) and Face-On (Cellulose I) Adsorption of Cellulose Nanocrystals at the Oil–Water Interface: A Combined Entropic and Enthalpic Process
Somia Haouache (Centre National de la Recherche Scientifique, Université de Poitiers), Yu Chen (Beijing Institute of Technology), Clara Jiménez-Saelices (Institut National de Recherche pour l'Agriculture, l'Alimentation et l'Environnement, Biopolymères Interactions Assemblages), Fabrice Cousin (Centre National de la Recherche Scientifique, Commissariat à l'Énergie Atomique et aux Énergies Alternatives), Pan Chen (Beijing Institute of Technology), Yoshiharu Nishiyama (Centre National de la Recherche Scientifique, Centre de Recherches sur les Macromolécules Végétales), François Jérôme (Centre National de la Recherche Scientifique, Université de Poitiers), Isabelle Capron (Institut National de Recherche pour l'Agriculture, l'Alimentation et l'Environnement, Biopolymères Interactions Assemblages)
Résumé : Nanocelluloses can be used to stabilize oil-water surfaces, forming so-called Pickering emulsions. In this work, we compare the organization of native and mercerized cellulose nanocrystals (CNC-I and CNC-II) adsorbed on the surface of hexadecane droplets dispersed in water at different CNC concentrations. Both types of CNCs have an elongated particle morphology and form a layer strongly adsorbed at the interface. However, while the layer thickness formed with CNC-I is independent of the concentration at 7 nm, CNC-II forms a layer ranging from 9 to 14 nm thick with increasing concentration, as determined using small-angle neutron scattering with contrast-matched experiments. Molecular dynamics (MD) simulations showed a preferred interacting crystallographic plane for both crystalline allomorphs that exposes the CH groups (100 and 010) and is therefore considered hydrophobic. Furthermore, this study suggests that whatever the allomorph, the migration of CNCs to the oil-water interface is spontaneous and irreversible and is driven by both enthalpic and entropic processes.