Biomimetic multiscale structure with hierarchically entangled topologies of cellulose-based hydrogel sensors for...

The development of high-performance cellulose-based sensors with superior interfacial compatibility, flexibility, and strength has always been challenging. Drawing inspiration from the intricate multiscale hierarchy found in resilient natural materials, the incorporation of this structure into cellulose-based hydrogels using biomimetic strategies is anticipated to enhance their properties. Therefore, the cellulose/polyacrylamide (PAM) hybrid hydrogels are fabricated using the aqueous AlCl₃/ZnCl₂ system through an all-green one-pot method at room temperature, achieving efficient dissolution of cellulose at multiple scales and in-situ polymerization of polyacrylamide. The multiscale cellulose/PAM hydrogels achieve good interfacial compatibility, with the reinforcing mechanism being confirmed through a combination of experimental validation and atomic simulations. The findings underscore the key elements that drive the multiscale behavior of hydrogels, encompassing a range of factors such as multiple interfacial interactions, hierarchical molecular entanglements, and microskeleton reinforcement. The hydrogels exhibit satisfactory stretchability (412 %), compressive strength (1.2 MPa), conductivity (1.65 S m^-1), and ultralong circulability (> 12,000 cycles), rendering them suitable for various scenarios of human-computer interaction. This work establishes a comprehensive interpretation of the strengthening mechanism in cellulose-based multiscale hierarchical structures, thereby providing novel insights for the advanced design strategies of other promising hierarchical materials.