Enhancing the Toughness of PAA/LCNF/SA Hydrogel through Double-Network Crosslinking for Strain Sensor Application

Lignin-containing nanocellulose fibers (LCNF) have been considered as a valuable enhancer for polyacrylic acid (PAA)-based hydrogels that can form rigid porous network structures and provide abundant polar groups. However, the PAA-LCNF hydrogel is dominated by a single-network (SN) structure, which shows certain limitations when encountering external environments with high loads and large deformations. In this paper, sodium alginate (SA) was introduced into the PAA-LCNF hydrogel network to prepare a double-network (DN) hydrogel structure of the SA-Ca²⁺ and PAA-LCNF through a two-step process. The covalent network of PAA-LCNF acts as the resilient framework of the hydrogel, while the calcium bridging networks of SA, along with the robust hydrogen bonding network within the system, function as sacrificial bonds that dissipate energy and facilitate stress transfer. The resulting hydrogel has porous morphologies. Results show that SA can effectively improve the mechanical properties of DN hydrogels and endow them with excellent thermal stability and electrical conductivity. Compared with pure PAA-LCNF hydrogel, the elongation at break of DN hydrogel increased from 3466% to 5607%. The good electrical conductivity makes it possible to use the flexible sensors based on DN hydrogel to measure electrophysiological signals. Our results can provide a reference for developing multifunctional hydrogels that can withstand ultra large deformation.