Aqueous zinc‐ion batteries (AZIBs) are an appealing battery system due to their low cost, intrinsic safety, and environmental‐friendliness, while their application is plagued by the obstacles from the cathode, electrolyte, and zinc anode. Summarizing the design principles and strategies toward the optimization of cathode, electrolyte, and zinc anode is crucial for the development of AZIBs. Herein, we present a comprehensive analysis of the design principles and promising strategies toward the improvement of AZIBs. Firstly, the various reaction mechanisms are summarized and the existing issues associated with the cathode, electrolyte, and zinc anode are discussed to guide the rational design of AZIBs. Subsequently, we provide an in‐depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization, and analyze the advantages and disadvantages of various strategies. Importantly, the design principles and strategies of the newly appeared conversion‐type AZIBs, such as Zn‐S battery and Zn‐Se battery, are also discussed and analyzed. The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail. Finally, some research trends and perspectives are provided for designing better AZIBs.

Transition metal phosphides, such as iron phosphide (FeP), have been considered as promising anode candidates for high-performance sodium ion batteries (SIBs) owing to their high theoretical capacity. However, the development of FeP is limited by large volume change, low electrical conductivity and sluggish kinetics with sodium ions. Moreover, the sodium storage kinetics and dynamics behavior in FeP are still unclear. Herein, improved sodium storage ability of FeP is achieved by volume regulation and surface engineering via a rationally designed hierarchical porous FeP@C/rGO nanocomposite. This FeP@C/rGO nanocomposite exhibits excellent rate capability and long cycle life as the anode of SIBs. Specifically, the FeP@C/rGO nanocomposite delivers high specific capacities of 635.7 and 343.1 mA h g⁻¹ at 20 and 2000 mA g⁻¹, respectively, and stable cycling with 88.2% capacity retention after 1000 cycles. The kinetics and dynamics studies demonstrate that the superior performance is attributed to the rationally designed hierarchical porous FeP@C/rGO with a high capacitive contribution of 93.9% (at 2 mV s⁻¹) and a small volume expansion of only 54.9% by in situ transmission electron microscopy (TEM) measurement. This work provides valuable insights into understanding the phase evolution of FeP during the sodiation/desodiation process for designing high-performance SIBs.

Lithium–sulfur (Li–S) batteries with high energy density and natural abundance are critical to achieve the low-cost and large-scale energy storage applications. Suffering from the sluggish redox kinetics together with the accumulated intermediate Li₂S_x (x = 4–8) polysulfides in the liquid electrolytes during charging/discharging, the high-performance Li–S batteries are stagnant by the issues such as high level of electrochemical irreversibility and poor cyclability. Herein, a bifunctional interlayer composed of metallic conductive NiCo₂S₄ nanosheets with large area and mesopores supported on carbon textile (NiCo₂S₄@CT) is fabricated for high-performance Li–S batteries. The mesoporous and metallic conductive NiCo₂S₄ nanosheets with large area not only provide strong chemical bonding for polysulfides, but also show efficient catalytic effect towards accelerating the polysulfide redox reactions. When served as an interlayer, NiCo₂S₄@CT endows the Li–S batteries with a high initial capacity of ∼1600 mA h g⁻¹ at 0.1C and ultra-stable cycling performance with a slow capacity decay rate of 0.018% per cycle over 500 cycles. The results proffer a facile and promising approach to design Li–S batteries with high rate performance and high reversible capacities.

A N-doped graphene microlattice aerogel fabricated by a 3D printing technology followed by N₂plasma treatment is employed as Na metal host. Experimental and calculation results show the sodiophilic site is mainly originated from pyrrolic-N defects.