Phosphoric acid-mediated green preparation of regenerated cellulose spheres and their use for all-cellulose cross-linked superabsorbent hydrogels.

With the growing environmental concerns and an emergent demand, a growing attention is turned to eco-friendly superabsorbent hydrogels instead of synthetic counterparts. Hydrogels based on cellulose derivatives can absorb and retain a huge amount of water in the interstitial sites of their structures, stimulating their uses in various useful industrial purposes. In this work, cross-linked superabsorbent composite hydrogel films (CHF) were designed, manufactured and characterized, by taking advantage of the combination of carboxymethyl cellulose (CMC), hydroxyethyl cellulose (HEC) and newly developed regenerated cellulose (RC) spheres. RC with sphere-like shape was successfully prepared using a green method based on cold phosphoric acid-mediated dissolution of microcrystalline cellulose (MCC) followed by regeneration process using water as anti-solvent. Prior to be used, the morphological and structural properties of RC spheres, with an average diameter of 477 ± 270 nm, were examined by SEM, AFM, XRD, FTIR and TGA techniques. CHF crosslinked with citric acid were, in fact, prepared by solvent casting method with different RC weight fractions (i.e. 0, 2.5, 5, 10 and 15 wt%), then the crosslinking reaction was triggered by thermal treatment at 80 °C during 8 h. Prepared CHF were then characterized in terms of their structural, thermal, tensile and transparency properties. Swelling tests were carried at three different aqueous media (i.e. with a pH = 3, 6.4 or 11) to evaluate the water retention capacity of hydrogel films, as well as, the pH effect on their swelling and hydrolytic degradation properties. Collected results reveal that CHF with low RC content (i.e. RC weight fraction of 2.5 or 5 wt%) have the best tensile and swelling properties, with a tensile strength and a swelling capacity (at pH = 6.4) up to 95 MPa and 4000%, respectively.