Ionogels are extremely soft ionic materials that can undergo large deformation while maintaining their structural and functional integrity. Ductile ionogels can absorb energy and resist fracture under external load, making them an ideal candidate for wearable electronics, soft robotics, and protective gear. However, developing high-modulus ionogels with extreme toughness remains challenging. Here, a facile one-step photopolymerization approach to construct an acrylic acid (AA)-2-hydroxyethylacrylate (HEA)-choline chloride (ChCl) eutectogel (AHCE) with ultrahigh modulus and toughness is reported. With rich hydrogen bonding crosslinks and phase segregation, this gel has a 99.1 MPa Young's modulus and a 70.6 MJ m −3 toughness along with 511.4% elongation, which can lift 12 000 times its weight. These features provide extreme damage resistance and electrical healing ability, offering it a protective and strain-sensitive coating to innovate anticutting fabric with motion detection for human healthcare. The work provides an effective strategy to construct robust ionogel materials and smart wearable electronics for intelligent life.
Conductive hydrogels promise great application prospects in future flexible sensor areas. However, great challenges remain in successfully constructing a green hydrogel sensor with efficient synergy from various advantages simultaneously using green starting chemicals via a one-step green procedure. In this work, these challenges were overcome via a superhydrogen-bond network (SHBN) strategy, by which a novel polyvinyl acetate/tannic acid/graphene oxide (PVA/TA/GO) hydrogel was readily constructed and successfully synergized robust mechanical properties (e.g., supporting an 80 kg boy) with strong anti-damage (a hydrogel with a pre-drilled hole was not fractured at 300% strain), anti-freezing (strong mechanical performance, good electrical conductivity, strain sensitivity and stable signal output capacity were retained even at extremely low temperatures when performing real-time tasks) and anti-drying ability (after exposure to air for three months, the hydrogel did not dry out and retained excellent mechanical/anti-freezing performance similar to that of the original hydrogel). The easy construction (one-step freezing) of the hydrogel and its significantly strengthened mechanical properties and excellent anti-freezing/anti-drying ability mainly result from the SHBNs between the hydroxyls on PVA and the hydroxyls on TA/GO/glycerol. Moreover, no toxic/volatile starting chemicals were used in the preparation or discharged into the surrounding environment. More attractively, the hydrogel possesses both cancer-killing ability and biocompatibility. Another impressive facet is that after being assembled into a hydrogel sensor, it can satisfactorily recognize various motion signals. Therefore, the SHBN strategy, which unites diverse outstanding advantages in a single material, opens up a new avenue for designing new high-performance hydrogels for application even in extremely low-temperature or dry environments.
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