A Self-Healing and Sweat-Chargeable Hydrogel Electrolyte for All-in-One Flexible Supercapacitors

Flexible solid-state supercapacitors (SCs) with hydrogel as an electrolyte and separator combine the advantages of wearability and energy storage and exhibit a broad application prospect in wearable energy textiles. However, irreversible electrolyte damage and unstable electrode-electrolyte interfaces during mechanical deformations remain bottlenecks in realizing truly wearable applications. Herein, poly(acrylic acid) (PAA)-Fe hydrogels were prepared through a simple thermal polymerization strategy. The dynamic reversible metal coordination bonds between Fe³⁺ and carboxylic acids confers the hydrogels with excellent self-healing properties. As expected, the prepared hydrogels exhibited superior mechanical strength (tensile stress of 45.80 kPa), ionic conductivity (0.076 S cm^-1), and self-healing properties. Subsequently, the SCs were constructed using composite hydrogel electrodes (MnO₂@CC embedded in the PAA-Fe hydrogels) as symmetrical electrodes (marked as MSCs). The reversible metal coordination bonds between composite hydrogel electrodes formed an ultrastable electrode/electrolyte interface in the all-in-one MSCs, thus revealing excellent mechanical durability. The all-in-one MSCs delivered a remarkable specific capacitance (30.98 F g^-1 at 0.2 A g^-1), excellent cyclic stability (87.24% after 5000 cycles), outstanding mechanical deformation stability, and impressive electrochemical output stability after self-healing (capacitance retention of 85.34% after five cycles of cutting/self-healing). It is noteworthy that the all-in-one MSCs employed NaCl as an electrolyte, which can be obtained from human sweat. As a proof of the self-charged concept, the all-in-one MSCs can be reused in sweat, whose capacitance was maintained at 90.05% of the initial state after three repetitions. This work is expected to shine light into the design of all-in-one and fabric-based SCs and the development of wearable energy textiles.