The uncontrollable growth of lithium (Li) dendrites and the instability of the Li/electrolyte interface hinder the development of nextgeneration rechargeable lithium metal batteries. The combination of inorganic nanoparticles and polymers as the artificial SEI layer shows great potential in regulating lithium-ion flux. Here, we design spatially confined LiF nanoparticles in an aligned polymer matrix as the artificial SEI layer. A high dielectric polymer matrix homogenizes the electric field near the surface of lithium metal. Aligned pores with LiF nanoparticles promote the lithium-ion transport across the artificial SEI layer. The synergistic effect of the highly polar β-phase PVDF and LiF nanoparticles provides high stability over 900 h for the Li//Li symmetrical cell. Besides, a Li//LFP full battery equipped with this artificial layer shows good performance in the commercial carbonate electrolyte, demonstrating the great potential of this protective film in lithium metal batteries.
Garnet‐type Li6.4La3Zr1.4Ta0.6O12 (LLZ) electrolyte is a promising candidate for high‐performance solid‐state batteries, while its applications are hindered by interfacial problems. Although the utilization of functional coatings and molten lithium (Li) effectively solves the LLZ interfacial compatibility problem with Li metal, it poses problems such as high cost, high danger, and structural damage. Herein, a mixed conductive layer (MCL) is introduced at the LLZ/Li interface (RT‐MCL) via an in situ cold bonding process at room temperature. Such a stable and compact RT‐MCL can effectively suppress side reactions and protect the crystal structure of LLZ, and it also inhibits growth of Li dendrites and promotes uniform Li deposition. The critical current density (CCD) of the Li symmetric cell composed of RT‐MCL‐LLZ is increased to 1.8 mA cm‐2 and provides stable cycling performance over 2000 h under 0.5 mA cm‐2. Additionally, this in situ cold bonding treatment can significantly reduce cost and eliminate potential safety issues caused by the high‐temperature processing of Li metal. This work highlights tremendous potential of this cold bonding technique in the reasonable design and optimization of the LLZ/Li interface.
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