Surface engineering of inorganic solid-state electrolytes via interlayers strategy for developing long-cycling quasi-all-solid-state lithium batteries

作者：Ju-Sik Kim, Gabin Yoon, Sewon Kim, Shoichi Sugata, Nobuyoshi Yashiro, S. Suzuki, Myung-Jin Lee, Ryounghee Kim, M. Badding, Zhen Song, Jaemyung Chang, D. Im · 发表于：Nature Communications · 年份：2023 · DOI：10.1038/s41467-023-36401-7 · 被引用次数：146 · 研究领域：Medicine

Lithium metal batteries (LMBs) with inorganic solid-state electrolytes suffer from lithium dendrites propagation. Here, the authors demonstrate the production of stable lab-scale LMBs using an Ag-coated Li_6.4La_3Zr_1.7Ta_0.3O_12 inorganic solid electrolyte in combination with a silver-carbon interlayer. Lithium metal batteries (LMBs) with inorganic solid-state electrolytes are considered promising secondary battery systems because of their higher energy content than their Li-ion counterpart. However, the LMB performance remains unsatisfactory for commercialization, primarily owing to the inability of the inorganic solid-state electrolytes to hinder lithium dendrite propagation. Here, using an Ag-coated Li_6.4La_3Zr_1.7Ta_0.3O_12 (LLZTO) inorganic solid electrolyte in combination with a silver-carbon interlayer, we demonstrate the production of stable interfacially engineered lab-scale LMBs. Via experimental measurements and computational modelling, we prove that the interlayers strategy effectively regulates lithium stripping/plating and prevents dendrite penetration in the solid-state electrolyte pellet. By coupling the surface-engineered LLZTO with a lithium metal negative electrode, a high-voltage positive electrode with an ionic liquid-based liquid electrolyte solution in pouch cell configuration, we report 800 cycles at 1.6 mA/cm^2 and 25 °C without applying external pressure. This cell enables an initial discharge capacity of about 3 mAh/cm^2 and a discharge capacity r...