Customising Sustainable Bio-Based Polyelectrolytes: Introduction of Charged and Hydrophobic Groups in Cellulose.

Cellulose has been widely explored as a sustainable alternative to synthetic polymers in industrial applications, thanks to its advantageous properties. The introduction of chemical modifications on cellulose structure, focusing on cationic and hydrophobic modifications, can enhance its functionality and expand the range of applications. In the present work, cationization was carried out through a two-step process involving sodium periodate oxidation followed by a reaction with the Girard T reagent, yielding a degree of substitution for cationic groups (DS(cationic)) between 0.3 and 1.8. Hydrophobic modification was achieved via esterification with fatty acids derived from commercial plant oils, using an enzyme-assisted, environmentally friendly method. Lipase-catalysed hydrolysis, optimised at 0.25% enzyme concentration and with a 1 h reaction time, produced an 84% yield of fatty acids, confirmed by FTIR and NMR analyses. The degree of substitution for hydrophobic groups (DS(hydrophobic)) ranged from 0.09 to 0.66. The molecular weight (MW) of the modified cellulose derivatives varied from 1.8 to 141 kDa. This dual modification strategy enables the creation of cellulose-based polymers with controlled electrostatic and hydrophobic characteristics, customisable for specific industrial applications. Our approach presents a sustainable and flexible solution for developing cellulose derivatives tailored to diverse industrial needs.