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The practical application of high‐energy lithium (Li) metal anodes is plagued by the severe issues of interfacial instability. The Li3N originated from the decomposition of LiNO3 is believed to endow the solid electrolyte interphase (SEI) with high stability and ionic conductivity. However, the precise control on the decomposition of LiNO3 is still challenging due to the sophisticated reaction pathways and high energy barriers. In this study, a self‐assembled monolayers (SAMs) with densely packed and long‐range ordered sulfonic acid groups on an alumina‐coated separator are designed. By providing a strong dipole moment, this SAMs efficiently facilitate the rapid and deep decomposition of LiNO3, leading to the formation of an SEI rich in Li3N nanocrystals. Notably, under the stringent conditions of 5 mA cm−2 and 5 mAh cm−2, the Li/Li symmetric cell is still able to cycle stably for 1000 h under the stable nitrided interface induced by the SAMs. Consequently, the application scenarios of SAMs technology in precisely controlling electrolyte decomposition processes are successfully expanded to stabilize the interphase of metallic Li anode with high energy‐density. [ABSTRACT FROM AUTHOR]

Recently emerging lithium ternary chlorides have attracted increasing attention for solid‐state electrolytes (SSEs) due to their favorable combination between ionic conductivity and electrochemical stability. However, a noticeable discrepancy in Li‐ion conductivity persists between chloride SSEs and organic liquid electrolytes, underscoring the need for designing novel chloride SSEs with enhanced Li‐ion conductivity. Herein, an intriguing trigonal structure (i.e., Li3SmCl6 with space group P3112) is identified using the global structure searching method in conjunction with first‐principles calculations, and its potential for SSEs is systematically evaluated. Importantly, the structure of Li3SmCl6 exhibits a high ionic conductivity of 15.46 mS cm−1 at room temperature due to the 3D lithium percolation framework distinct from previous proposals, associated with the unique in‐plane cation ordering and stacking sequences. Furthermore, it is unveiled that Li3SmCl6 possesses a wide electrochemical window of 0.73−4.30 V vs Li+/Li and excellent chemical interface stability with high‐voltage cathodes. Several other Li3MCl6 (M = Er, and In) materials with isomorphic structures to Li3SmCl6 are also found to be potential chloride SSEs, suggesting the broader applicability of this structure. This work reveals a new class of ternary chloride SSEs and sheds light on strategy for structure searching in the design of high‐performance SSEs. [ABSTRACT FROM AUTHOR]

Uneven lithium (Li) metal deposition typically results in uncontrollable dendrite growth, which renders an unsatisfactory cycling stability and coulombic efficiency (CE) of Li metal batteries (LMBs), preventing their practical application. Herein, a novel carbon cloth with the modification of ZnO nanosheets (ZnO@CC) is fabricated for LMBs. The as‐prepared ZnO@CC with a cross‐linked network significantly reduces the local current density, and the design of ZnO nanosheets can promote the uniform deposition of Li metal as lithiophilic sites. As a result, the Li metal anodes (LMAs) based on ZnO@CC (ZnO@CC@Li) enables a long cycle life over 640 hours with a low overpotential of 65 mV at a current density of 4 mA cm−2 with a capacity of 1 mAh cm−2 in the symmetric cell. Moreover, when coupling the ZnO@CC@Li with a LiFePO4 cathode, the assembled full cell exhibits excellent long cycle and rate performance, highlighting its promising practical application prospect. [ABSTRACT FROM AUTHOR]

Rechargeable zinc-based batteries are expected to be the next generation energy storage system because of their high specific capacity, low redox potential, low cost, eco-friendliness, and abundant reserves. Nevertheless, their large-scale applicability is restricted due to water-induced side reactions, and the uneven plating/stripping of Zn on the anodes. Herein, an artificial protective layer acting as a desolvation layer and a zinc ion flux regulator is proposed for the reconstruction of the Zn/electrolyte interface and to promote the formation of an ultra-even amorphous solid–electrolyte interface (SEI) on Zn metal. As a consequence, the modified Zn anode displays a strong zincophilic property and decreasing interfacial impedance. The artificial layer obtained can inhibit the side reactions and induce the uniform deposition of zinc ions to avoid Zn dendrite formation in the charge/discharge process. With this advantage, the dendrite-free Zn anode exhibits a higher cycling stability (over 1200 h at 2 mA cm−2) than that of the bare Zn anode. This is also confirmed in the full Zn‖V2O5 battery with an ultrahigh discharge capacity after 1000 cycles. [ABSTRACT FROM AUTHOR]