Controlled Polyelectrolyte Association of Chitosan and Carboxylated Nano-Fibrillated Cellulose by Desalting

We prepared chitosan (CHI) hydrogels reinforced with highly charged cellulose nanofibrils (CNF) by the desalting method. To this end, the screening of electrostatic interactions between CHI polycation and CNF polyanion was performed by adding NaCl at 0.4 mol/L to the chitosan acetate solution and to the cellulose nanofibrils suspension. The polyelectrolyte complexation between CHI polycation and CNF polyanion was then triggered by desalting the CHI/CNF aqueous mixture by multistep dialysis, in large excess of chitosan. Further gelation of non-complexed CHI was performed by alkaline neutralization of the polymer, yielding high reinforcement effects as probed by the viscoelastic properties of the final hydrogel. The results showed that polyelectrolyte association by desalting can be achieved with a polyanionic nanoparticle partner. Beyond obtaining hydrogel with improved mechanical performance, these composite hydrogels may serve as precursor for dried solid forms with high mechanical properties.

Automated summary

In this study, chitosan hydrogels were prepared using the desalting method, with cellulose nanofibrils serving as reinforcement. Through multiple-step dialysis desalting, polyelectrolyte complexation between chitosan and cellulose nanofibrils was achieved. The resulting hydrogels showed enhanced mechanical properties and potential for use as precursors for high-strength solid forms.