Ti₃C₂T_xMXene-Activated Fast Gelation of Stretchable and Self-Healing Hydrogels: A Molecular Approach

MXene-based hydrogels, a flourishing family of soft materials, have recently emerged as promising candidates for stretchable electronics. Despite recent progress, most works use MXenes as conductive nanofillers. Herein, by tuning the molecular interactions between MXene nanosheets and other constituents within the hydrogels, we demonstrate Ti3C3Tx MXene can act as a versatile cross-linker to activate the fast gelation of a wide range of hydrogels, starting from various monomer- and polymer-based precursors. The gelation behavior varies significantly across hydrogels. In general, the fast gelation mechanism is attributed to the easier generation of free radicals with the help of Ti3C2Tx MXene and the presence of multiscale molecular interactions between MXene and polymers. The use of MXene as a dynamic cross-linker leads to superior mechanical properties, adhesion, and self-healing ability. Owing to the inherent photothermal behavior of Ti3C3Tx and the heterogeneous phase-transforming features of polymers, a polymer-MXene hydrogel is demonstrated to exhibit distinctive thermosensation-based actuation upon near-infrared illumination, accompanied by rapid shape transformation.