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

As one important component of sulfur cathodes, the carbon host plays a key role in the electrochemical performance of lithium-sulfur (Li-S) batteries. In this paper, a mesoporous nitrogen-doped carbon (MPNC)-sulfur nanocomposite is reported as a novel cathode for advanced Li-S batteries. The nitrogen doping in the MPNC material can effectively promote chemical adsorption between sulfur atoms and oxygen functional groups on the carbon, as verifi ed by X-ray absorption near edge structure spectroscopy, and the mechanism by which nitrogen enables the behavior is further revealed by density functional theory calculations. Based on the advantages of the porous structure and nitrogen doping, the MPNC-sulfur cathodes show excellent cycling stability (95% retention within 100 cycles) at a high current density of 0.7 mAh cm −2 with a high sulfur loading (4.2 mg S cm −2 ) and a sulfur content (70 wt%). A high areal capacity (≈3.3 mAh cm −2 ) is demonstrated by using the novel cathode, which is crucial for the practical application of Li-S batteries. It is believed that the important role of nitrogen doping promoted chemical adsorption can be extended for development of other high performance carbon-sulfur composite cathodes for Li-S batteries.

Nitrogen-Doped Mesoporous Carbon Promoted Chemical Adsorption of Sulfur and Fabrication of High-Areal-Capacity Sulfur Cathode with Exceptional Cycling Stability for Lithium-Sulfur Batteries

Potassium-ion batteries (PIBs) have attracted tremendous attention due to their low cost, fast ionic conductivity in electrolyte, and high operating voltage. Research on PIBs is still in its infancy, however, and achieving a general understanding of the drawbacks of each component and proposing research strategies for overcoming these problems are crucial for the exploration of suitable electrode materials/electrolytes and the establishment of electrode/cell assembly technologies for further development of PIBs. In this review, we summarize our current understanding in this field, classify and highlight the design strategies for addressing the key issues in the research on PIBs, and propose possible pathways for the future development of PIBs toward practical applications. The strategies and perspectives summarized in this review aim to provide practical guidance for an increasing number of researchers to explore next-generation and high-performance PIBs, and the methodology may also be applicable to developing other energy storage systems.

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Approaching high-performance potassium-ion batteries via advanced design strategies and engineering.

Li-ion batteries (LIBs), commercialized in 1991, have the highest energy density among practical secondary batteries and are widely utilized in electronics, electric vehicles, and even stationary energy storage systems. Along with the expansion of their demand and application, concern about the resources of Li and Co is growing. Therefore, secondary batteries composed of earth-abundant elements are desired to complement LIBs. In recent years, K-ion batteries (KIBs) have attracted significant attention as potential alternatives to LIBs. Previous studies have developed positive and negative electrode materials for KIBs and demonstrated several unique advantages of KIBs over LIBs and Na-ion batteries (NIBs). Thus, besides being free from any scarce/toxic elements, the low standard electrode potentials of K/K+ electrodes lead to high operation voltages competitive to those observed in LIBs. Moreover, K+ ions exhibit faster ionic diffusion in electrolytes due to weaker interaction with solvents and anions than that of Li+ ions; this is essential to realize high-power KIBs. This review comprehensively covers the studies on electrochemical materials for KIBs, including electrode and electrolyte materials and a discussion on recent achievements and remaining/emerging issues. The review also includes insights into electrode reactions and solid-state ionics and nonaqueous solution chemistry as well as perspectives on the research-based development of KIBs compared to those of LIBs and NIBs.

Research Development on K-Ion Batteries.

Finding a viable electrolyte for next-generation 5 V-class lithium-ion batteries is of primary importance. A long-standing obstacle has been metal-ion dissolution at high voltages. The LiPF6 salt in conventional electrolytes is chemically unstable, which accelerates transition metal dissolution of the electrode material, yet beneficially suppresses oxidative dissolution of the aluminium current collector; replacing LiPF6 with more stable lithium salts may diminish transition metal dissolution but unfortunately encounters severe aluminium oxidation. Here we report an electrolyte design that can solve this dilemma. By mixing a stable lithium salt LiN(SO2F)2 with dimethyl carbonate solvent at extremely high concentrations, we obtain an unusual liquid showing a three-dimensional network of anions and solvent molecules that coordinate strongly to Li(+) ions. This simple formulation of superconcentrated LiN(SO2F)2/dimethyl carbonate electrolyte inhibits the dissolution of both aluminium and transition metal at around 5 V, and realizes a high-voltage LiNi0.5Mn1.5O4/graphite battery that exhibits excellent cycling durability, high rate capability and enhanced safety.

Superconcentrated Electrolytes for a High-Voltage Lithium-Ion Battery

Graphite as an anode for the potassium ion battery (PIBs) has the merits of low cost and potentially high energy density, while suffering from limited cycle time and inferior stability. Herein we, using a concentrated electrolyte, demonstrate that formation of a robust inorganic-rich passivation layer on the graphite anode could resolve these problems. Consequently, the PIBs with graphite anode could operate for over 2000 cycles (running time of over 17 months) with negligible capacity decay, and had a high area capacity over 7.36 mAh cm-2 with a high mass loading of 28.56 mg cm-2 . These unprecedented performances of graphite are comparable to that of traditional lithium-ion batteries, and may promote the rapidly development of high performance PIBs.

Graphite Anode for a Potassium-Ion Battery with Unprecedented Performance

A low cost nonaqueous potassium-based battery-supercapacitor hybrid device (BSH) is successfully established for the first time with soft carbon as the anode, commercialized activated carbon as the cathode, and potassium bis(fluoro-slufonyl)imide in dimethyl ether as the electrolyte. This BSH reconciles the advantages of potassium ion batteries and supercapacitors, achieving a high energy density of 120 W h kg-1 , a high power density of 599 W kg-1 , a long cycle life of 1500 cycles, and an ultrafast charge/slow discharge performance (energy density and power density are calculated based on the total mass of active materials in the anode and cathode). This work demonstrates a great potential of applying the nonaqueous BSH for low cost electric energy storage systems.

A Nonaqueous Potassium‐Based Battery–Supercapacitor Hybrid Device

Potassium-organic batteries have a great potential for applications in the grid-scale energy storage owing to their low cost and abundant resources, although they suffer from the inferior cycle stability, fast capacity decay, and low power density. A highly reversible phase transformation of the organic cathode during potassiation/depotassiation is the key factor for the capacity retention, as revealed here. Consequently, the potassium-organic battery achieves a high power density of 9796 W kg-1 , a remarkable energy efficiency of 89%, a long cycle stability for 1000 cycles, a superior areal capacity around 2 mA h cm-2 , and a long-term cycling time over 8 months. Besides, the full cells also exhibit a superior rate performance and good cycle stability over 3000 cycles. This work provides new insight into the stabilization of the organic cathode, and demonstrates the enormous potential of organic cathodes for application in high-power potassium-ion batteries (PIBs), which may bring PIBs to new heights.

An Ultrafast and Highly Stable Potassium-Organic Battery.

Potassium ion-batteries (PIBs) have attracted tremendous attention recently due to the abundance of potassium resources and the low standard electrode potential of potassium. Particularly, the solid-electrolyte interphase (SEI) in the anode of PIBs plays a vital role in battery security and battery cycling performance due to the highly reactive potassium. However, the SEI in the anode for PIBs with traditional electrolytes is mainly composed of organic compositions, which are highly reactive with air and water, resulting in inferior cycle performance and safety hazards. Herein, a highly stable and effective inorganic SEI layer in the anode is formed with optimized electrolyte. As expected, the PIBs exhibit an ultralong cycle performance over 14 000 cycles at 2000 mA g-1 and an ultrahigh average coulombic efficiency over 99.9%.

Ruifang Ma

Papers

Graphite Anode for a Potassium-Ion Battery with Unprecedented Performance

A Nonaqueous Potassium‐Based Battery–Supercapacitor Hybrid Device

An Ultrafast and Highly Stable Potassium-Organic Battery.

Ultrastable Potassium Storage Performance Realized by Highly Effective Solid Electrolyte Interphase Layer.

Covalent sulfur for advanced room temperature sodium-sulfur batteries