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

Ju-Sik Kim (), Gabin Yoon, Sewon Kim, Shoichi Sugata, Nobuyoshi Yashiro, Shinya Suzuki, Myung-Jin Lee, Ryounghee Kim, Michael Badding, Zhen Song, JaeMyung Chang and Dongmin Im ()
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Ju-Sik Kim: Battery Material Lab., Samsung Advanced Institute of Technology, 130, Samsung-ro, Yeongtong-gu
Gabin Yoon: Battery Material Lab., Samsung Advanced Institute of Technology, 130, Samsung-ro, Yeongtong-gu
Sewon Kim: Battery Material Lab., Samsung Advanced Institute of Technology, 130, Samsung-ro, Yeongtong-gu
Shoichi Sugata: Samsung R&D Institute Japan, Samsung Electronics, 2-1-11, Semba Nishi, Minoh
Nobuyoshi Yashiro: Samsung R&D Institute Japan, Samsung Electronics, 2-1-11, Semba Nishi, Minoh
Shinya Suzuki: Samsung R&D Institute Japan, Samsung Electronics, 2-1-11, Semba Nishi, Minoh
Myung-Jin Lee: Battery Material Lab., Samsung Advanced Institute of Technology, 130, Samsung-ro, Yeongtong-gu
Ryounghee Kim: Battery Material Lab., Samsung Advanced Institute of Technology, 130, Samsung-ro, Yeongtong-gu
Michael Badding: Sullivan Park Campus, Corning Incorporated
Zhen Song: Sullivan Park Campus, Corning Incorporated
JaeMyung Chang: Sullivan Park Campus, Corning Incorporated
Dongmin Im: Battery Material Lab., Samsung Advanced Institute of Technology, 130, Samsung-ro, Yeongtong-gu

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract 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 Li6.4La3Zr1.7Ta0.3O12 (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/cm2 and 25 °C without applying external pressure. This cell enables an initial discharge capacity of about 3 mAh/cm2 and a discharge capacity retention of about 85%.

Date: 2023
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DOI: 10.1038/s41467-023-36401-7

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