Flexible All-in-one Quasi-Solid-State Batteries Enabled by Low-water-content Hydrogel Films

The high conductivities and good mechanical properties of hydrogel electrolyte films are critical for energy storage devices with high flexibility, fast redox kinetics, and long life. Herein, a low water content (6.63 wt%) hydrogel film is prepared, and a favorable environment is created, with an electrochemical stability window of 2.26 V and a high ionic conductivity of 2.6 mS cm^-1 . The hydrogel film exhibits good folding ability, low in-plane swelling, and anti-freezing abilities. These properties are benefitted by immobilizing free water molecules on the abundant oxygenic groups of polymer fibers in the hydrogel film, offering a unique 3D channel to allow Li⁺ to quickly transport along the polymer network. Therefore, the hydrogel film-based all-in-one flexible cell exhibits stable cycling performance with a retention of 81.8% of the initial capacity after 500 cycles at room temperature and 66.2% of capacity retention at -30 °C. Furthermore, the full cell with high cathode loading (≈21 mg cm^-2 ) exhibits a high areal capacity of 2.5 mAh cm^-2 (≈119 mAh g^-1 ). The overall merits of flexible all-in-one quasi-solid-state batteries demonstrate high potential to be used for power wearable electronics.