| Summary: | Modification of cellulosic-rich materials for the production of cellulose-based polyelectrolytes (PELs) can bring several benefits, such as high biodegradability and low or no toxicity, for numerous applications, when compared with the use of traditional, synthetic PELs. Moreover, cellulose-based PELs originating from wood wastes, contribute to the valorisation of such wastes. In this work, <i>Eucalyptus</i> pulps with diverse lignin contents, extracted from <i>Eucalyptus</i> wood wastes, were anionized by a two–step reaction procedure (periodate oxidation followed by sulfonation). Applying different reaction times (24–144 h) in the sulfonation step allowed for producing a range of cellulose-based anionic polyelectrolytes with different characteristics. PELs obtained after 24 and 72 h of sulfonation were thoroughly characterized (Fourier transform infrared and <sup>1</sup>H nuclear magnetic resonance spectroscopies, zeta potential and degree of substitution (elemental analysis) and hydrodynamic diameter (dynamic light scattering)) and subsequently evaluated as flocculants in decolouration processes of model effluents (Methylene Blue and Crystal Violet) and an industrial effluent from a textile industry. Furthermore, possible flocculation mechanisms induced by the use of the various PELs are discussed. Results are compared with those obtained with a commonly applied, synthetic flocculant (polyacrylamide). It is demonstrated that it was possible to obtain water-soluble lignocellulosic PELs starting from raw materials with different degrees of purity and that those PELs are promising eco-friendly alternative flocculation agents for the decolouration of effluents.
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