A Novel Polyacrylamide Composite Hydrogel Reinforced with Deep Eutectic Solvent-Pretreated Paulownia Cellulose/Nanocellulose: Preparation, Characterization and Properties

Biomass represents a vital and sustainable resource for developing renewable materials with the potential to replace petroleum-based chemicals. Paulownia wood has high cellulose content and a loose wood structure, giving it natural advantages as a biomass material. Therefore, in this study, Paulownia wood was selected as a lignocellulosic feedstock. An integrated pretreatment process combining a deep eutectic solvent (DES) with an organic solvent was employed to efficiently remove lignin and hemicellulose, yielding cellulose-enriched residues. Subsequently, high-intensity ultrasonication was applied to convert the residues into cellulose nanofibers and nanocrystals. Using the extracted cellulose and nanocellulose, a dual-crosslinked network composite hydrogel was fabricated. The structural, mechanical, thermal, swelling, and conductive properties of the hydrogel were systematically investigated. The results show that, compared with the blank group hydrogel, the addition of nanocellulose increased the maximum tensile strength and tensile strain of the composite hydrogel by approximately 113% and 81%, respectively; meanwhile, the compressive strengths of the nanocellulose-based hydrogels (0.04575–0.09060 MPa) are higher than that of the blank group hydrogel (0.04235 MPa), confirming that the incorporation of nanocellulose significantly enhances the mechanical strength and elasticity of the hydrogel. The introduction of an AlCl3/ZnCl2 solvent system imparts appreciable electrical conductivity. Furthermore, the composite hydrogel maintains structural integrity after full swelling, indicating good dimensional stability and reusability. This work not only presents a green and efficient strategy for valorizing Paulownia biomass but also offers a novel design route for high-performance conductive hydrogel materials, highlighting their potential application in areas such as flexible electronics and energy storage.