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Supramolecular systems based on chitosan and cellulose nanofibers (CNFs) with a different surface modification (TEMPO-oxidation and carboxymethylation) were investigated and utilized for the functional consolidation of paper. Prior to the paper consolidation, the interactions between chitosan and CNFs dispersed in aqueous solvent were studied. It was detected that the peculiar surface functionalization of nanocellulose is crucial to control the chitosan/CNFs electrostatic attractions and, consequently, the entropic/enthalpic contributions and the stoichiometry of the biopolymer adsorption onto the cellulose nanofibers. Dynamic Light Scattering and rheological experiments revealed that the presence of biopolymeric chains on the CNFs surface favors the entanglement and the aggregation between the nanofibers reinforcing their network. It was observed that chitosan and nanocellulose exhibit synergetic effects on the paper consolidation in terms of reinforcing action, surface hydrophobization and enhancement of the fire-resistance. In conclusion, this paper demonstrates that the electrostatic interactions between chitosan and functionalized nanocellulose drive the formation of hybrid fillers suitable for paper consolidation. Chitosan coated CNFs possess an improved capacity to penetrate the paper structure causing an enhancement of the mechanical resistance and surface hydrophobization. Moreover, chitosan/CNFs create a protective barrier for heat transfer that prevents the paper combustion.

A novel material for the deacidification and protection of paper has been designed by using MgO filled halloysite nanotubes (Hal). The ability of MgO loaded nanotubes to control the acidic conditions was evaluated by pH measurements in aqueous solvent. Afterwards, paper was impregnated into hydroxypropyl cellulose dispersions containing the consolidating material. A simulation of strong acidic conditions allowed us to evaluate the deacidification effect of the composite material on the samples. In particular, the paper reaches a pH of 7.7 after 1 h exposition to HNO 3 vapours when MgO-Hal nanoparticles are added to the impregnation mixture at a concentration of 10 wt% and it remains still neutral after 12 h. Dynamic mechanical analysis showed that the tensile strength of the consolidated paper is improved, since the stress at breaking increase of ca. 8% for the samples treated with MgO-Hal compared to the untreated paper. Due to the presence of halloysite loaded with the alkaline reservoir, the acidic degradation of cellulose is neutralized as suggested by the stored energy which is similar to the pristine paper without any chemical attack. Therefore, the mechanical performances of the paper are preserved during the aging together with its macroscopic aspect, as suggested by colorimetric analysis. The proposed consolidation protocol represents a further step for the self-healing and long-term protection of cellulose based artworks. [Display omitted] • MgO was loaded within halloysite nanotubes (Hal) by electrostatic interactions. • Paper was treated using hydroxypropyl cellulose/MgO-Hal aqueous dispersions. • MgO-Hal act as deacidifying fillers of cellulose. • The morphology, pH and tensile properties of the treated paper were investigated. • Treatment by 10 wt% MgO-Hal provides a paper protection from acidic aging. [ABSTRACT FROM AUTHOR]