The dendritic issue in aqueous zinc‐ion batteries (ZBs) using neutral/mild electrolytes has remained an intensive controversy for a long time: some researchers assert that dendrites severely exist while others claim great cycling stability without any protection. This issue is clarified by investigating charge/discharge‐condition‐dependent formation of Zn dendrites. Lifespan degradation (120 to 1.2 h) and voltage hysteresis deterioration (134 to 380 mV) are observed with increased current densities due to the formation of Zn dendrites (edge size: 0.69–4.37 µm). In addition, the capacity is also found to remarkably affect the appearance of the dendrites as well. Therefore, at small current densities or loading mass, Zn dendrites might not be an issue, while the large conditions may rapidly ruin batteries. Based on this discovery, a first‐in‐class electrohealing methodology is developed to eliminate already‐formed dendrites, generating extremely prolonged lifespans by 410% at 7.5 mA cm–2 and 516% at 10 mA cm–2. Morphological analysis reveals that vertically aligned Zn dendrites with sharp tips gradually become passivated and finally generate a smooth surface. This developed electrohealing strategy may promote research on metal dendrites in various batteries evolving from passive prevention to active elimination, rescuing in‐service batteries in situ to achieve elongated lifetime.
Working voltage substantially limits the practical applications of batteries. This review emphasizes on the voltage issue of aqueous metal-ion batteries.
Hydrogel materials are receiving increasing research interest due to their intriguing structures that consist of a crosslinked network of polymer chains with interstitial spaces filled with solvent water. This feature endows the materials with the characteristics of being both wet and soft, making them ideal candidates for electrolyte materials for flexible energy storage devices, such as supercapacitors and rechargeable batteries that are under intensive studies nowadays. More importantly, the highly abundant and tunable chemistries of these hydrogels allow the introduction of novel functionalities into the existing hydrogels so that it is possible to fabricate unprecedented energy storage devices with additional functions. Here, the state-of-the-art advances of the hydrogel materials for flexible energy storage devices including supercapacitors and rechargeable batteries are reviewed. In addition, devices with various kinds of functions, such as self-healing, shape memory, and stretchability, are also included to stress the critical role of hydrogel materials. Furthermore, the challenges embedded in the current technologies are also highlighted and discussed with the hope to continually boost future research for the fast-developing field.
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