Zinc-ion batteries are promising power sources, but their practical application is impeded by the Zn dendrite growth and side reactions at the electrode/electrolyte interface. Here, we report that such issues can be effectively addressed by a self-healable hydrogel electrolyte. The electrolyte is comprised of carboxyl-modified poly­(vinyl alcohol) cross-linked by COO–Fe bonding in the presence of Zn­(NO3)2 and MnSO4. A quasi-solid-state Zn–MnO2 battery using the electrolyte delivers a specific capacity up to 177 mAh g–1 after 1000 cycles with a retention rate of 83%, which is much better than its equivalent using an aqueous electrolyte. The improvement is attributed to efficient suppression of the dendrite growth and side reactions at the electrode/electrolyte by the hydrogel electrolyte. More importantly, the battery autonomously recovery its energy-storage functions even after multiple physical damages, showing excellent robustness and reliability. The present investigation provides an effective strategy to address the energy-storage performance and reliability of a light-metal battery system.

Poor stability is a long-standing problem preventing the practical application of Li metal anodes, which is fundamentally attributed to their fragile solid electrolyte interphase (SEI) layers that are intrinsically neither adaptable to the dynamic volume change nor self-healable after breakage. Here a Li metal anode is effectively stabilized by in situ integrating its SEI layer into a self-healable polydimethylsiloxane (PDMS) network cross-linked via imine bonding. The self-healing network enables the integrated SEI layer to readily accommodate the volume change but also to repair itself after breaking. Consequently, the resulting anode exhibits excellent cycling stability and a dendrite-free morphology. In a Li/LiFePO4 full cell, this strategy leads to capacity retention up to 99% and a Coulombic efficiency >99.5% after 300 cycles. Our investigation provides a novel self-healing strategy for developing stable Li-metal anodes aiming at high energy-density batteries.

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Reliability and safety are critical issues for portable power sources aiming for next-generation electronics. However, most lithium-ion batteries (LIBs) will fail to work or will cause safety problems after physical damage or violent deformation. Here, an omni-healable aqueous LIB, which can self-repair its electrodes and electrolyte simultaneously after mechanical breakage, is fabricated by integrating all of the electroactive components into polymer networks cross-linked by dynamic borate ester bonding. Once suffering from repeated cutoffs, the battery quickly recovers its configuration integrity as well as mechanical and electrochemical properties autonomously without external stimuli. Furthermore, the battery can also be tailored into complicated patterns while maintaining its lithium-storage properties. The present investigation offers a strategy to design a smart and sustainable energy-storage device that has potential applications in wearable/flexible electronics, flexible robot or intelligent apparel, and so on.

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