Microstructure-controlled Li ion conductive oxide–based ceramic solid electrolytes supporting high current densities

作者：Nataly Carolina Rosero‐Navarro, Haruna Watanabe, Randy Jalem, Maycol F. Mena, Xinhao Yang, Shota Sugio, Hiroaki Ito, Yoshitaka Tateyama, Akira Miura, Kiyoharu Tadanaga · 发表于：Electrochimica Acta · 年份：2025 · DOI：10.1016/j.electacta.2025.146233 · 被引用次数：5 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Thermal Expansion and Ionic Conductivity

The fabrication of all-solid-state batteries using lithium metal that can be operated at high current densities (free lithium dendrites) is a recognized worldwide goal. We used a glassy lithium borate (LBO)–based microstructure as the grain boundary modifier of a garnet-type solid electrolyte to prevent lithium dendrite formation at high current densities. The relative density (90 %) and ionic conductivity (10 –4 S cm –1 ) were similar for LBO-modified and non-modified solid electrolytes. Notably, a post-annealing step at 175 °C significantly reduces the interfacial resistance between the LBO-modified electrolyte and lithium metal. LBO in the solid electrolyte microstructure distributes the current and prevents dendrite propagation, suppressing lithium dendrites up to 10 mA cm –2 . Low voltage response at a current density of 10 mA cm –2 for 60 galvanostatic plating–stripping cycles establishes the fast-charging capability of this composite electrolyte. Density functional theory calculations reveal that LBO offers a broader electrochemical stability window compared to LLZ, enhancing overall stability within the 0–3.4 V range. This work provides a promising route to simultaneously achieve high current density operation and improved interfacial stability in garnet-based solid-state batteries, accelerating the practical implementation of lithium-metal anodes.