Abstract
The construction of ionic conductive hydrogels with high transparency, excellent mechanical robustness, high toughness, and rapid self-recovery is highly desired yet challenging. Herein, a hydrogen-bonding network densification strategy is presented for preparing a highly stretchable and transparent poly(ionic liquid) hydrogel (PAM-r-MVIC) from the perspective of random copolymerization of 1-methyl-3-(4-vinylbenzyl) imidazolium chloride and acrylamide in water. Ascribing to the formation of a dense hydrogen-bonding network, the resultant PAM-r-MVIC exhibited an intrinsically high stretchability (>1000%) and compressibility (90%), fast self-recovery with high toughness (2950 kJ m−3), and excellent fatigue resistance with no deviation for 100 cycles. Dissipative particle dynamics simulations revealed that the orientation of hydrogen bonds along the stretching direction boosted mechanical strength and toughness, which were further proved by the restriction of molecular chain movements ascribing to the formation of a dense hydrogen-bonding network from mean square displacement calculations. Combining with high ionic conductivity over a wide temperature range and autonomous adhesion on various surfaces with tailored adhesive strength, the PAM-r-MVIC can readily work as a highly stretchable and healable ionic conductor for a capacitive/resistive bimodal sensor with self-adhesion, high sensitivity, excellent linearity, and great durability. This study might provide a new path of designing and fabricating ionic conductive hydrogels with high mechanical elasticity, high toughness, and excellent fatigue resilience for skin-inspired ionic sensors in detecting complex human motions.
Highlights
A skin-inspired ionic sensor is widely concerned in the generation of smart wearable electronics for the applications of artificial intelligence, human-machine interfaces, healthcare monitoring, and soft robotics [1,2,3]
The real-time response of an ionic sensor is realized through the directional migration of ions in an ionic conductor under deformation, which can realize the integrated functions of high elasticity and skin comparable modulus that are difficult to realize in a traditional electronic conductor
Hydrogen bonds between the amino groups among the AM structure and the 3-N atoms among the methyl-3-(4-vinylbenzyl) imidazolium chloride (MVIC) structure were achieved among the PAM-r-MVIC
Summary
A skin-inspired ionic sensor is widely concerned in the generation of smart wearable electronics for the applications of artificial intelligence, human-machine interfaces, healthcare monitoring, and soft robotics [1,2,3]. Due to its high mechanical elasticity, high ionic conductivity, good transparency (close to 100% in visible light range), and excellent self-adhering properties, the PAM-r-MVIC can readily work in a resistive/capacitive bimodal sensor, showing high sensitivity, wide response range, and excellent stability in real-time monitoring of large-strain movements (i.e., finger and wrist bending) and small-strain movements (i.e., swallowing) of complex human motions This newly developed hydrogen-bonding network densification strategy for the design and construction of functional ionic conductive hydrogels provides new ideas for the development of ionic skin sensors with high mechanical elasticity, good transparency, self-adhering property, and excellent durability in a wide temperature range
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