The ever‐growing demands for electrical energy storage have stimulated the pursuit of alternative advanced batteries. Zn‐ion batteries (ZIBs) are receiving increased attentions due to the low cost, high safety, and high eco‐efficiency. However, it is still a big challenge to develop suitable cathode materials for intercalation of Zn ions. This review provides a timely access for researchers to the recent activities regarding ZIBs. First, cathode materials including various manganese oxides, vanadium compounds, and Prussian blue analogs are summarized with details in crystal structures and Zn ion storage mechanisms. Then, the electrolytes and their influences on the electrochemical processes are discussed. Finally, opinions on the current challenge of ZIBs and perspective to future research directions are provided.

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Recent Advances in Zn-Ion Batteries

Although current high-energy-density lithium-ion batteries (LIBs) have taken over the commercial rechargeable battery market, increasing concerns about limited lithium resources, high cost, and insecurity of organic electrolyte scale-up limit their further development. Rechargeable aqueous zinc-ion batteries (ZIBs), an alternative battery chemistry, have paved the way not only for realizing environmentally benign and safe energy storage devices but also for reducing the manufacturing costs of next-generation batteries. This Review underscores recent advances in aqueous ZIBs; these include the design of a highly reversible Zn anode, optimization of the electrolyte, and a wide range of cathode materials and their energy storage mechanisms. We also present recent advanced techniques that aim at overcoming the current issues in aqueous ZIB systems. This Review on the future perspectives and research directions will provide a guide for future aqueous ZIB study.

Recent Advances in Aqueous Zinc-Ion Batteries

Zinc-ion batteries built on water-based electrolytes featuring compelling price-points, competitive performance, and enhanced safety represent advanced energy storage chemistry as a promising alternative to current lithium-ion battery systems. Attempts to develop rechargeable aqueous zinc-ion batteries (ZIBs) can be traced to as early as the 1980s; however, since 2015, the research activity in this field has surged throughout the world. Despite the achievements made in exploring electrode materials so far, significant challenges remain at the material level and even on the whole aqueous ZIBs system, leading to the failure of ZIBs to meet commercial requirements. This review aims to discuss how to pave the way for developing aqueous ZIBs. The current research efforts related to aqueous ZIBs electrode materials and electrolytes are summarized, including an analysis of the problems encountered in both cathode/anode materials and electrolyte optimization. Some concerns and feasible solutions for achieving practical aqueous ZIBs are discussed in detail. We would like to point out that merely improving the electrode materials is not enough; synergistic optimization strategies toward the whole battery system are also deeply needed. Finally, some perspectives are provided on the subsequent optimization design for further research efforts in the aqueous ZIB field.

Issues and opportunities facing aqueous zinc-ion batteries

Aqueous zinc ion batteries (ZIBs) are truly promising contenders for the future large-scale electrical energy storage applications due to their cost-effectiveness, environmental friendliness, intri...

Active Materials for Aqueous Zinc Ion Batteries: Synthesis, Crystal Structure, Morphology, and Electrochemistry

Advanced rechargeable zinc-based batteries: Recent progress and future perspectives

DOI: 10.1002/aenm.201702463 other secondary batteries.[6–8] However, LIBs are too expensive to scale up for the processing cost resulted from the limited lithium resources, and SIBs are subjected to complicated issues of safety as well as environmental issues.[9–12] So, it is an urgent challenge for exploring new energy storage systems. As an alternative, rechargeable aqueous Zn-ion batteries (ZIBs) have received incremental attention owing to the following advantages, including low cost, safety, and environmentally friendly.[13] Meanwhile, using aqueous electrolyte to replace the organic electrolyte is of great significance for reducing the cost and environmental pollution.[14] However, it is difficult to find suitable cathode material as the host for the intercalation of Zn2+ owing to the high polarization of Zn2+ as well as the narrow applicable voltage range, which is limited by the water splitting in the aqueous battery system.[15] Typically, polymorphs of MnO2 (α-, γ-phase) are highly attractive as the cathode material because of the tunnel structure suiting for the intercalation of Zn2+ and a matched potential within the stable range of water. Some results, based on the reversible intercalation of Zn2+, have been reported in recent years, and they show either limited specific capacity or poor cycling performance.[16–19] Recently, the MnO2 nanofiber electrode, reported by Liu and co-workers, shows high capacity and excellent cycling performance.[20] However, the rate performance is not high enough due to the sluggish reaction dynamics of conversion reaction. Prussian blue analogues, including of zinc hexacyanoferrate and copper hexacyanoferrate, are another class of cathode materials, which show limited specific capacity as well as poor cyclic stability.[21–23] Until very recently, vanadiumbased materials are explored for reversible Zn2+ intercalation.[24] Nazar and co-workers reported a bilayered Zn0.25V2O5·nH2O cathode, which shows a high-capacity and long-life performance.[25] However, the development of ZIBs is in the primary stage, some new cathode materials should also be explored to enhance the energy density as well as cycle life for ZIBs. Over the past decades, layered vanadium oxides have been applied as electrode materials for LIBs or SIBs due to their low cost and high capacities.[26,27] Generally, the bulk vanadium oxides suffer from a rapid capacity fading resulting from low electronic conductivity, poor structural stability during the ion de/intercalation.[28] Recent studies show that interlayer metal ions (MxVnOm, M = metal ion) can act as pillars to increase the Aqueous Zn-ion batteries (ZIBs) have received incremental attention because of their cost-effectiveness and the materials abundance. They are a promising choice for large-scale energy storage applications. However, developing suitable cathode materials for ZIBs remains a great challenge. In this work, pioneering work on the designing and construction of aqueous Zn//Na0.33V2O5 batteries is reported. The Na0.33V2O5 (NVO) electrode delivers a high capacity of 367.1 mA h g−1 at 0.1 A g−1, and exhibits long-term cyclic stability with a capacity retention over 93% for 1000 cycles. The improvement of electrical conductivity, resulting from the intercalation of sodium ions between the [V4O12]n layers, is demonstrated by single nanowire device. Furthermore, the reversible intercalation reaction mechanism is confirmed by X-ray diffraction, Raman, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy analysis. The outstanding performance can be attributed to the stable layered structure and high conductivity of NVO. This work also indicates that layered structural materials show great potential as the cathode of ZIBs, and the indigenous ions can act as pillars to stabilize the layered structure, thereby ensuring an enhanced cycling stability. Zinc Ion Batteries

Sodium Ion Stabilized Vanadium Oxide Nanowire Cathode for High-Performance Zinc-Ion Batteries

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Sodium Ion Stabilized Vanadium Oxide Nanowire Cathode for High-Performance Zinc-Ion Batteries