Rechargeable aqueous zinc-ion batteries (AZIBs) have captured a surge of interest in recent years as a promising alternative for scalable energy storage applications owing to the intrinsic safety, affordability, environmental benignity, and impressive electrochemical performance. Despite the facilitated development of this technology by many investigations, however, its smooth implementation is still plagued by inadequate energy density and undesirable life span, which calls for an efficient and controllable cathode storage chemistry. Here, this review focuses on the key bottlenecks by offering a comprehensive summary of representative cathode materials and comparatively analyzing their structural features and electrochemical properties. Then, we critically present several feasible electrode design strategies to guide future research activities from a fundamental perspective for high-energy-density and durable cathode materials mainly in terms of interlayer regulation, defect engineering, multiple redox reactions, activated two-electron reactions, and electrochemical activation and conversion. Finally, we outline the remaining challenges and future perspectives of developing high-performance AZIBs.

Vanadium-based compounds with an open framework structure have become the subject of much recent investigation into aqueous zinc-ion batteries (AZIBs) due to high specific capacity. However, there are some issues with vanadium dissolution from a cathode framework as well as the generation of byproducts during discharge that should not be ignored, which could cause severe capacity deterioration and inadequate cycle life. Herein, we report several barium vanadate nanobelt cathodes constructed of two sorts of architectures, i.e., Ba 1., which are controllably synthesized by tuning the amount of barium precursor. Benefiting from the robust architecture, layered Ba x V 3 O 8 -type nanobelts (Ba 1.2 V 6 O 16 •3H 2 O) exhibit superior rate capability and long-term cyclability owing to fast zinc-ion kinetics, enabled by efficiently suppressing cathode dissolution as well as greatly eliminating the generation of byproduct Zn 4 SO 4 (OH) 6 •xH 2 O, which provides a reasonable strategy to engineer cathode materials with robust architectures to improve the electrochemical performance of AZIBs.

Rechargeable aqueous zinc-ion batteries have shown great potential for grid-scale applications owing to their high safety, low cost and sustainability.

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