Energy Dissipation Mediated by Multiple Noncovalent Interactions in Hydrogen‐Bonded Organic Frameworks‐Based Hydrogels for Wearable Gesture‐to‐Recognition Translation

Abstract Hydrogels hold great promises in intelligent wearable gesture‐to‐recognition translation devices, but high mechanical robustness usually encounters low sensitivity and poor cycling stability, it is pivotal and challenging to balance energy dissipation and conductivity. Herein, the soft‐hard multiphase hydrogels have been proposed for the first time through noncovalently threading polymerizable deep eutectic solvent (PDES) into hydrogen‐bonded organic frameworks (HOFs). Fluorine groups on HOF (HOF‐F) are presented as the hydrogen bond acceptors to form multiple noncovalent interactions between HOF‐F and PDES, which expedites the energy dissipation with synchronous increment of ion transport in hydrogels. The tensile strength, toughness and ionic conductivity are as high as 135.23 kPa, 2.69 MJ m −3 and 4.33 ± 0.02 S m −1 , respectively, which greatly outperforms that of H‐substituted counterpart (60.04 kPa, 0.75 MJ m −3 and 3.74 ± 0.08 S m −1 ) and ranks the top in the reported hydrogels. The resultant hydrogel sensor achieves high sensitivity of 2.2 and remarkable cyclic stability over 1000 cycles, thus accurately monitoring human motion and recognizing the gesture. This work provides a promising approach to develop smart flexible electronics.