Strong
mechanical performance, appropriate adhesion capacity, and
excellent biocompatibility of conductive hydrogel-based sensors are
of great significance for their application. However, conventional
conductive hydrogels usually exhibit insufficient mechanical strength
and adhesion. In addition, they will lose flexibility and conductivity
under subzero temperature and a dry environment owing to inevitable
freezing and evaporation of water. In this study, a tough, flexible,
self-adhesive, long-term moisturizing, and antifreezing organohydrogel
was prepared, which was composed of gelatin, zwitterionic poly [2-(methacryloyloxy)
ethyl] dimethyl-(3-sulfopropyl) (PSBMA), MXene nanosheets, and glycerol.
Natural gelatin was incorporated to enhance mechanical performance
via the entanglement of a physical cross-linked network and a PSBMA
network, which was also used as a stabilizer to disperse MXene into
the organohydrogel. Zwitterionic PSBMA endowed the organohydrogel
with good adhesion and self-healing properties. Long-term moisturizing
properties and antifreeze tolerance could be achieved owing to the
synergistic water retention capacity of PSBMA and glycerol. The resulting
PSBMA–gelatin–MXene–glycerol (PGMG) organohydrogel
exhibited high mechanical fracture strength (0.65 MPa) and stretchability
(over 1000%), excellent toughness (3.87 MJ/m3), strong
and repeated adhesion to diverse substrates (e.g., paper, glass, silicon
rubber, iron, and pig skin), good fatigue resistance (under the cyclic
stretching–releasing process), and rapid recovery capacity.
Moreover, the PGMG organohydrogel showed good stability under −40
°C. The sensor based on PGMG organohydrogel could tightly attach
to the human skin and real-time-monitor the motions of joints (e.g.,
bending of the finger, wrist, elbow, and knee) and the change in mood
such as smiling and frowning. Therefore, PGMG organohydrogels have
a huge potential for wearable sensors under room temperature or extreme
environments.