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Solid polymer electrolytes can be used to construct solid-state lithium batteries (SSLBs) using lithium metals as the anode. However, the lifespan and safety problems of SSLBs caused by lithium dendrite growth have hindered their practical application. Here, we have designed and prepared a rigid-flexible asymmetric solid electrolyte (ASE) that is used in building SSLBs. The ASE can inhibit efficiently the growth of lithium dendrites and lead to a long cycle life of SSLBs due to the hierarchical structure of a combination of “polymer-in-ceramic” (i.e., rigid ceramic layer of Li6.4La3Zr1.4Ta0.6O12) and “LiBOB-in-polymer” (i.e., soft polymer-layer of polyethylene oxide and LiBOB components). The results demonstrated that a symmetrical battery with ASE (Li|ASE|Li) can be steadily cycled for more than 2000 h and yielded a flat plating/stripping voltage profile under a current density of 0.1 mA cm–2. As a consequence, the SSLB of LiFePO4|ASE|Li delivered a specific capacity of 155.1 mA h g–1 with a capacity retention rate up to 90.2% after 200 cycles with the Coulombic efficiency over 99.6% per cycle. This asymmetric structure combines the advantages of ceramics and polymers, providing an ingenious solution for building rigid and flexible solid electrolytes.

Based on the analysis of systematic research (density functional theory calculations, physical characterizations, and electrochemical performances), here, we report a novel mixture surface modification layer of LiC6&LiF, which can enhance the lithium-ion diffusion and decrease the local current density. This is beneficial to the improvement of cycling stability. As a result, the Li@LiC6&LiF-5/NCM half-cell possesses an excellent capacity retention of 94% after 100 cycles at 0.1C, with a capacity decay of only 0.06% per cycle. For comparison, the capacity retention of a pristine Li/NCM cell is only 9.3% after 100 cycles. Our study confirms that compositing the high ionic conductivity layer (e.g., LiC6&LiF for the first time) is a promising avenue to stabilize lithium-metal anodes. From this perspective, we concisely review recent discoveries in this field and suggest possible new research directions for further development of Li-metal batteries.

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