Rheological study of hybrid aqueous suspension of TEMPO-oxidized cellulose nanofibrils and graphene oxide

The incorporation of graphene oxide (GO) into a nanocellulose matrix has attracted considerable attention due to the unique advantages of both components. This study focuses on investigating the viscoelastic and flow properties of hybrid aqueous suspensions (2.00 w/v%), composed of TEMPO-oxidized cellulose nanofibrils (TOCNF) and GO at different TOCNF/GO weight ratios. To adjust the elastic properties of the hybrid suspensions, calcium ions are introduced, varying the concentration systematically to study their effects on the hybrid network structure. All blends exhibit shear-thinning behaviour and demonstrate elastic, gel-like properties. Notably, in the absence of calcium ions, the enhancement of elastic properties is more pronounced at higher GO fractions. Conversely, with the introduction of calcium ions, the enhancement of elastic properties becomes particularly important at higher TOCNF fractions. For the quantitative evaluation of these enhancements, we employ the logarithmic mixing rule. Significant positive deviations from the predictions of the logarithmic mixing rule are ascribed to the complex, concentration-dependent arrangement of cellulose nanofibrils and GO liquid crystals in the aqueous suspension, coupled with ionic crosslinking induced by calcium ions. The study aims to contribute to the understanding of the rheological behaviour of the TOCNF/GO hydrogel, showing potential advancements in various applications.

Graphical abstract