Stretchable,
healable, biocompatible, and conductive hydrogels
are one of the promising candidates for both wearable electronics
and environmental remediation applications. To date, the design of
hydrogels that integrate ultrafast self-healing with high efficiency
(seconds), high stretchability, and biocompatibility and reversibility
into one system is not an easy task. Herein, we demonstrate a general
oxidation approach to accelerate the hydrogelation of hPEI-based double
network gels via the generation of fluorescent polymer clusters at
room temperature or triggered by the heating–cooling process.
The resulting ohPEI hydrogel has the merit of biocompatibility over
most reported hPEI hydrogels for strain sensors. It shows a high conductivity
(1.3 S/m), an ultrafast self-healing ability (<3 s, 98% healing
efficiency within 60 s), a high stretchability (∼1850 and ∼7000%
in deformation), and reversible adhesivity on various material surfaces.
The excellent performance of the hydrogel is ascribed to the cooperative
and hierarchical interactions of four types of dynamic combinations,
including the reversible borate bond, hydrogen bonding, electrostatic
interaction, and polymer cluster interactions. The reversible fabrication
process by the one-spot method (just by simple mixing of the components)
and superior properties of the hydrogel make it an ideal candidate
for a wearable strain sensor to monitor human motions and physiological
activities. Moreover, it is also a good hydrogel absorbent for phase
separation absorption of volatile organic compounds with a high capacity
(for acetone: 4.75 g g–1), reusability, and an easy
handling process.