Li metal has been intensively investigated as a next-generation rechargeable battery anode. However, its practical application as the anode material is hindered by the deposition of dendritic Li. To suppress dendritic Li growth, introducing a modified separator is considered an effective strategy since it promotes a uniform Li ion flux and strengthens thermal and mechanical stability. Herein, we present a strategy for the surface modification of separator, which involves coating the separator with a piezoelectric material (PM). The PM-coated separator shows higher thermal resistance than the pristine separator, and its modified surface properties enable the homogeneous regulation of the Li-ion flux when the separator is punctured by Li dendrite. Furthermore, PM was synthesized in different solvents via solvothermal method to explore the size effect. This strategy would be helpful to overcome the intrinsic Li metal anode problems.

Stabilizing the cubic phase of Li7La3Zr2O12 (LLZO) through doping has been a challenging issue, as conventional aliovalent dopants often decrease Li ion mobility and induce unwanted phase transformations. In this study, a novel multi-component doping strategy is proposed that stabilizes the cubic phase of LLZO while maintaining high Li ion mobility. The practical isovalent ions and their combinations are screened using density-functional theory (DFT) calculations and ab-initio molecular dynamics (AIMD) simulations, identifying the most stable multi-component alloy configuration that can stabilize the robust cubic phase of LLZO. Our results demonstrate that the proposed Li7La3(Zr, Hf, Ce, Ru)2O12 composition has a stable cubic phase at low temperatures, which we validated through experimental synthesis. Our proposed doping strategy has the potential to advance the development of high-performance all-solid-state batteries.

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