Oxygen-Vacancy-Engineered Biomimetic Interphase for Dendrite-Free Lithium-Metal Anodes.

The commercialization of lithium-metal batteries (LMBs) is severely hindered by uncontrolled lithium dendrite growth and poor interfacial stability. Here, we designed a biomimetic artificial solid electrolyte interphase that synchronizes physicochemical regulation to ensure interfacial stability and uniform lithium deposition. A patterned Li0.33La0.56TiO₃ (PL) nanofiber membrane with a uniform grid structure is fabricated via electrospinning and calcination. This unique architecture homogenizes Li⁺ flux and regulates the local current density, enabling uniform Li⁺ deposition and effective dendrite suppression. Furthermore, the introduction of oxygen vacancies into the black PL (BPL) lattice through in situ reduction significantly enhances the Li⁺ transport kinetics by lowering the migration energy barrier. As a result, the BPL@Li symmetric cells demonstrate exceptional cycling stability over 1400 h, and the BPL@Li||LiFePO₄ full cells retain 85% of its initial capacity after 200 cycles at 1 C, markedly outperforming bare lithium counterparts. This work offers a scalable and multifunctional interface engineering strategy toward high-performance LMBs.