In plant cell walls, xylan chains present various substituents including acetate groups. The influence of the acetyl substitution on the organization of xylan-cellulose complexes remains poorly understood. This work combines in vitro and in silico approaches to decipher the functional role of acetyl groups on the xylan/cellulose interaction. Acetylated xylans were extracted from apple pomace with dimethyl sulfoxide-lithium chloride (DMSO-LiCl) and deacetylated using a mild alkali treatment. The adsorption behavior of acetylated and deacetylated xylan fractions was investigated using quartz crystal microbalance with dissipation (QCM-D) and molecular dynamics. Acetylated xylans form a dense and poorly hydrated and rigid layer on cellulose with xylan chains that have two residues per helical turn conformation, whereas the deacetylated fraction forms a swollen and more viscous layer in which only the xylan chains in direct contact with the cellulose surface have two residues per helical turn conformation. The other chains have three residues per turn conformation.
Cellulose nanocrystals (CNC) and xyloglucan (XG) were used to construct new aerogels inspired by the hierarchical organization of wood tissue, i.e., anisotropic porous cellular solid with pore walls containing oriented and stiff cellulose nanorods embedded in hemicellulose matrix. Aerogels with oriented or disordered pores were prepared by directional and non-directional freeze-casting from colloidal dispersions of XG and CNC at different ratios. XG addition induced a clear improvement of the mechanical properties compared to the CNC aerogel, as indicated by the Young modulus increase from 138 kPa to 610 kPa. The addition of XG changed the pore morphology from lamellar to alveolar and it also decreased the CNC orientation (the Hermans' orientation factor was 0.52 for CNC vs 0.36-0.40 for CNC-XG). The aerogels that contained the highest proportion of XG also retained their structural integrity in water without any chemical modification. These results open the route to biobased water-resistant materials by an easy and green strategy based on polymer adsorption rather than chemical crosslinking.
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