The development of lithium metal anodes for next generation batteries remains a challenge. Uncontrolled Li dendrite growth not only induces severe safety issues but also leads to capacity fading by continuously consuming the electrolyte. This study demonstrates the design and fabrication of a composite protective layer composed of a high dielectric polymer, inorganic particles, and an electrolyte to overcome these obstacles. This layer not only suppresses dendrite growth, but also prevents LiPF6 degradation. The electrolyte introduced in the protective layer remains within the coating layer after solvent removal and acts as an ion transport channel at the interface. This enables the protective layer to exhibit high ionic conductivity and mechanical strength. The composite protective layer, which exhibits synergistic soft‐rigid characteristics, is placed on the Li metal anode and facilitates superior interfacial stability during long‐term cycles. LiMn2O4/coated lithium full cells using the composite protective layer show a superior rate capability and enhanced capacity retention compared to the cells using a bare lithium anode. The proposed strategy opens new avenues to fabricate a sustainable composite protective layer that affords superior performance in lithium metal batteries.
The future of next-generation rechargeable batteries, such as lithium metal, lithium−sulfur, and lithium−oxygen batteries, hinges on the utilization of metallic lithium as the anode. However, the practical application of lithium anodes has been challenging thus far due to the uncontrolled growth of lithium dendrites and extremely unstable interfaces between lithium and the electrolyte. Extensive investigations have been conducted to mitigate these limitations; nevertheless, there is a lack of fundamental insight into physical and chemical characteristics, the effect of thickness, and surface morphology of lithium anodes. Herein, an overview of the fundamental understanding of the effect of the shape of surface reliefs on lithium anode under the different cycling conditions is reported. Two different types of 10 μm deep surface reliefs, viz., continuous and discontinuous, were fabricated via soft lithography. It was newly found that the lithium-stripping behavior was significantly affected by the shape of surface reliefs. Furthermore, it is demonstrated that a 10 μm deep surface relief can not only be utilized on a thin lithium anode (20 μm) but also enhances the cell cycling stability. It is anticipated that the results will shed light on the practical utilization of lithium anodes by using the combination of other physical or chemical modification techniques.
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