Solid-state and liquid-free stretchable ionic conductors are highly desirable for stretchable electronics, because the ion-conductive hydrogels and ionogels suffer from potential solvent evaporation and leakage, respectively. Herein, we report a...
It remains a challenge to fabricate healable and recyclable polymeric materials with simultaneously enhanced tensile strength, stretchability, and toughness. Herein, we report a simple approach to fabricate high-performance polymer hydrogels that not only integrate high tensile strength, stretchability, and toughness but also possess selfhealing and recycling capabilities. The polymer hydrogels are fabricated by mixing a positively charged polyelectrolyte mixture of poly(diallyldimethylammonium chloride) (PDDA)/branched poly(ethylenimine) (PEI) with a negatively charged polyelectrolyte mixture of poly(sodium 4styrenesulfonate) (PSS)/poly(acrylic acid) (PAA) in an aqueous solution followed by molding, drying, and rehydration. The (PDDA/PEI)−(PSS/PAA) hydrogels with in situ-formed PDDA−PSS nanoparticles have a tensile strength, strain at break, and toughness of 1.26 ± 0.06 MPa, 2434.2 ± 150.3%, and 19.53 ± 0.48 MJ/m 3 , respectively. The toughness of the (PDDA/PEI)− (PSS/PAA) hydrogels is ∼5.2 and ∼108 times higher than that of the PEI−PAA and PDDA−PSS hydrogels, respectively. Benefiting from the high reversibility of the hydrogen-bonding and electrostatic interactions, the (PDDA/PEI)−(PSS/PAA) hydrogels can efficiently heal from physical damage to restore their original mechanical properties at room temperature in water. Moreover, the (PDDA/PEI)−(PSS/PAA) hydrogels after being dried and ground can be recycled under a pressure of ∼3 kPa at room temperature in the presence of water to reuse the damaged hydrogels.
In this work, self-healing
and recyclable polymer hydrogels with
simultaneously enhanced mechanical strength and stretchability are
fabricated through the complexation of poly(acrylic acid) (PAA) with
complexes of branched poly(ethylenimine) and 1-pyrenybutyric acid
(PEI-PYA) to generate PAA/PEI-PYA complexes, which are further molded,
dried, and rehydrated. The in situ-formed PYA nanofibrils with aggregated
structures during the complexation process enable the simultaneous
enhancement of the tensile strength and stretchability of the PAA/PEI-PYA
hydrogels. The PAA/PEI-PYA hydrogels have a tensile strength of 1.13
± 0.04 MPa and stretchability of 2970 ± 154%, which are
2.2 and 2.1 times higher than those of the PAA/PEI hydrogels. Meanwhile,
the damaged PAA/PEI-PYA hydrogels can be efficiently healed or recycled
at room temperature to regain their original mechanical strength and
integrity because the dynamic nature of hydrogen-bonding and electrostatic
interactions among PAA, PEI, and PYA endows the hydrogels with excellent
healing and recycling capacity. This strategy of using aggregated
nanofibrils to simultaneously enhance the tensile strength and stretchability
of hydrogels can be extended to PAA/PEI hydrogels reinforced with
aggregated nanofibrils of 9-anthracenecarboxylic acid and N,N′-di(propanoic acid)-perylene-3,4,9,10-tetracarboxylic
diimide, demonstrating its generality for fabricating hydrogels with
enhanced mechanical properties.
Due to the superior processability as well as readily-regulated mechanical and interfacial properties, polymer electrolytes are promising alternatives to inorganic solid electrolytes for lithium metal batteries (LMBs). However, polymer electrolytes...
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