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Aqueous zinc‐ion batteries (AZIBs), recognized for their safety and environmental friendliness, hold significant promise for large‐scale energy storage. However, the rapid capacity degradation resulting from the dissolution of active cathode materials hampers the advancement of AZIBs. Here, Ru0.2V2O5∙0.41H2O (RuVO) is synthesized with remarkable capacity retention (98.2% over 5000 cycles at 10 A g−1). The pre‐intercalation of Ru3+ enhances the stability of both intrinsic and cycling structures, elevating the Gibbs free energy and suppressing V‐dissolution thermodynamically. Additionally, Ru3+ intercalation modulates the potential energy surface of Zn2+ migration, leading to the dominance of Zn2+ in the insertion/extraction mechanism, thereby kinetically impeding the dissolution reaction. This study elucidates the dissolution thermodynamics and kinetics of V‐based cathodes through a combination of experiments, mechanism analyses, and density functional theory (DFT) calculations. [ABSTRACT FROM AUTHOR]

Lithium nitrate is an attractive lithium additive in the construction of high‐performance lithium metal anodes with a Li3N‐rich solid electrolyte interphase (SEI) layer. However, the eight‐electron transfer process induces high energy barriers between LiNO3 and Li3N. Herein, the inner Helmholtz plane is tuned on a Li deposition host to attain sluggish/rapid LiNO3 decomposition kinetics, resulting in different intermediate content distributions of Li species in the SEI. Notably, lithium oxynitride (LiNO) is identified as the decomposition intermediate, and experimental and simulation results confirm its role in obstructing LiNO3 decomposition. Moreover, the results reveal that the dipole–dipole interaction between LiNO and the polar V≡N bond can change the ionic/covalent character of the N═O bonds, considerably facilitating the energy transfer process of the N═O cleavage, and promoting a LiNO3 reduction to achieve a Li3N‐rich SEI. Consequently, when the electrolyte contains 0.37 m LiNO3, dendrite, and dead Li formation are suppressed effectively with the VN system, and an average Coulombic efficiency of 99.7% over 1000 cycles (1 mA cm−2, 1 mAh cm−2) can be attained. These results can promote the nitride oxidation break process and pave the way for fabricating high‐performance Li3N‐rich lithium metal batteries. [ABSTRACT FROM AUTHOR]

The simultaneous optimization of sluggish reaction kinetics and mass transfer in bifunctional oxygen electrocatalysts for air cathodes remains a great challenge. This study utilizes CoAl‐layered double hydroxide as a metal precursor to fabricate a bifunctional oxygen electrocatalyst, denoted as CoAlOXD‐Thin. This electrocatalyst features a specific core–shell structure of Co species, which grows on an aerophilic and conductive substrate composed of Al2O3 and carbon. It is successfully demonstrated that the thickness of Co@Co3O4 core–shell structure can be easily controlled by selecting different precursors and the combination of Co core and Co3O4 shell optimizes the adsorption strength of intermediates, leading to enhanced catalytic performance. Additionally, the Al species plays a dual role. It not only facilitates the mass transfer of oxygen species but also hinders the 2e− pathway of oxygen reduction reaction, leading to improved selectivity. Notably, the Zn–air batteries utilizing CoAlOXD‐Thin demonstrate an impressive peak power density of 216.2 mW cm−2, a high specific capacity of 800.8 mAh gZn−1, and excellent cycling stability and reversibility, surpassing those of the Pt/C + RuO2 catalyst. This study presents a novel approach to enhance air cathode performance by optimizing reaction kinetics and mass transfer through precursor design. [ABSTRACT FROM AUTHOR]

For wide and safe applications of Li metal batteries, the suppression of Li dendrite growth during cycling is the most crucial yet challenging topic. In this work, an artificial protective interlayer of GO‐BQ@LiTFSI (GBL) is designed to overcome this issue. The GBL interlayer is prepared by incorporating graphene‐oxide sheets with a liquid organic eutectic mixture of 1,4‐benzoquinone and bis (trifluoromethane) sulfonamide lithium salt. With the exceptional merits of these functional materials, the incorporation endows the GBL interlayer with rich lithiophilic active sites, good ionic conductivity, superior thermal stability and compatibility with the electrolyte, and the precursor supply stations for the formation of a compact and LiF‐rich solid‐electrolyte interface (SEI). Consequently, the GBL effectively promotes the uniform nucleation of Li at low over‐potentials and regulates the Li‐ion flux, leading to the formation of planar Li metal. After utilizing the GBL interlayer in the Li||Li symmetric cells, high electrochemical stability for 600 h is achieved at a current density of 3 mA cm−2 and a capacity of 3 mAh cm−2. Remarkably, this modification enables Li||LiFePO4 full cells with 1600 cycles at 1C and a high‐capacity retention of 95.23% with a cathode mass loading of ≈6 mg cm−2. [ABSTRACT FROM AUTHOR]