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.
In this paper, we propose the design of a family of hydrogel electrolytes that featuring freezing resistance, flexibility, safety, superior ionic conductivity and long-term stability to realize anti-freezing flexible aqueous batteries.
While α-MnO2 has been intensively studied for
zinc batteries, δ-MnO2 is usually believed to be
more suitable for ion storage with its layered structure. Unfortunately,
the extraordinary Zn ion storage performance that δ-MnO2 should exhibit has not yet been achieved due to the frustrating
structural degradation during charge–discharge cycles. Here,
we found the Na ion and water molecules pre-intercalation can effectively
activate stable Zn ion storage of δ-MnO2. Our results
reveal that the resulted Zn//pre-intercalated δ-MnO2 battery delivers an extraordinarily high-rate performance, with
a high capacity of 278 mAh g–1 at 1 C and up to
20 C, and a high capacity of 106 mAh g–1 can still
be measured. The capacity retention is as high as 98% after charged–discharged
up to 10,000 cycles benefiting from smooth Zn ion diffusion in the
pre-intercalated structure. Further
in situ
/ex situ characterization confirms the
superfast Zn ion diffusion in the pre-intercalated structure at room
temperature. In addition, utilizing the well-chosen electrode material
and modified polyurethane shell, we fabricated a quasi-solid-state
healable Zn-δ-MnO2, which can be self-healed after
multiple catastrophic damages, emphasizing the advanced features of
aqueous Zn ion battery for wearable applications.
Emerging research toward next-generation flexible and wearable electronics has stimulated the efforts to build highly wearable, durable, and deformable energy devices with excellent electrochemical performances. Here, we develop a high-performance, waterproof, tailorable, and stretchable yarn zinc ion battery (ZIB) using double-helix yarn electrodes and a cross-linked polyacrylamide (PAM) electrolyte. Due to the high ionic conductivity of the PAM electrolyte and helix structured electrodes, the yarn ZIB delivers a high specific capacity and volumetric energy density (302.1 mAh g and 53.8 mWh cm, respectively) as well as excellent cycling stability (98.5% capacity retention after 500 cycles). More importantly, the quasi-solid-state yarn ZIB also demonstrates superior knittability, good stretchability (up to 300% strain), and superior waterproof capability (high capacity retention of 96.5% after 12 h underwater operation). In addition, the long yarn ZIB can be tailored into short ones, and each part still functions well. Owing to its weavable and tailorable nature, a 1.1 m long yarn ZIB was cut into eight parts and woven into a textile that was used to power a long flexible belt embedded with 100 LEDs and a 100 cm flexible electroluminescent panel.
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