Lignin-modified cellulose nanofibers hydrogel under adjustable binary solvent systems with excellent adhesion, self-healing and anti-freeze properties

Hydrogels with remarkable flexibility have gained popularity as materials for current research. However, the unfavorable properties of short-term adhesion, susceptibility to damage, and freezing in low-temperature presented by conventional hydrogels have become bottlenecks for further applications. In this work, an anti-freezing hydrogel with excellent mechanical, adhesion, and self-healing properties were developed by constructing a persistent semiquinone/quinone-catechol redox equilibrium environment. The introduction of lignin-modified cellulose nanofibers (LCNFs) significantly improved the overall mechanical properties of the material, driven by strong hydrogen bond interactions. This enhancement was evident in the tensile properties (97.74 ± 1.72 kPa, 783 %) and compression properties (> 90 %). Within the internal network of the gel, the synergistic action of lignin and ammonium persulfate resulted in the production of catechol, which imparted the gel with excellent adhesion properties (28.26 ± 2.13 KPa) and broad adhesion applicability. In addition, the incorporation of ethylene glycol (EG) positively contributed to the strengthening of the gel while endowed with tunable anti-freezing properties. Given the exceptional advantages of the prepared hydrogels, they were used to assemble flexible strain sensors with outstanding sensitivity for monitoring human motions.