High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility

Sewon Kim, Ju-Sik Kim (), Lincoln Miara, Yan Wang, Sung-Kyun Jung, Seong Yong Park, Zhen Song, Hyungsub Kim, Michael Badding, JaeMyung Chang, Victor Roev, Gabin Yoon, Ryounghee Kim, Jung-Hwa Kim, Kyungho Yoon, Dongmin Im () and Kisuk Kang ()
Additional contact information
Sewon Kim: Seoul National University
Ju-Sik Kim: Samsung Advanced Institute of Technology
Lincoln Miara: Samsung Semiconductor, Inc.
Yan Wang: Samsung Semiconductor, Inc.
Sung-Kyun Jung: Samsung Advanced Institute of Technology
Seong Yong Park: Samsung Advanced Institute of Technology
Zhen Song: Sullivan Park Campus, Corning Incorporated
Hyungsub Kim: Korea Atomic Energy Research Institute
Michael Badding: Sullivan Park Campus, Corning Incorporated
JaeMyung Chang: Sullivan Park Campus, Corning Incorporated
Victor Roev: Samsung Advanced Institute of Technology
Gabin Yoon: Samsung Advanced Institute of Technology
Ryounghee Kim: Samsung Advanced Institute of Technology
Jung-Hwa Kim: Samsung Advanced Institute of Technology
Kyungho Yoon: Seoul National University
Dongmin Im: Samsung Advanced Institute of Technology
Kisuk Kang: Seoul National University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Lithium metal batteries using solid electrolytes are considered to be the next-generation lithium batteries due to their enhanced energy density and safety. However, interfacial instabilities between Li-metal and solid electrolytes limit their implementation in practical batteries. Herein, Li-metal batteries using tailored garnet-type Li7-xLa3-aZr2-bO12 (LLZO) solid electrolytes is reported, which shows remarkable stability and energy density, meeting the lifespan requirements of commercial applications. We demonstrate that the compatibility between LLZO and lithium metal is crucial for long-term stability, which is accomplished by bulk dopant regulating and dopant-specific interfacial treatment using protonation/etching. An all-solid-state with 5 mAh cm−2 cathode delivers a cumulative capacity of over 4000 mAh cm−2 at 3 mA cm−2, which to the best of our knowledge, is the highest cycling parameter reported for Li-metal batteries with LLZOs. These findings are expected to promote the development of solid-state Li-metal batteries by highlighting the efficacy of the coupled bulk and interface doping of solid electrolytes.

Date: 2022
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DOI: 10.1038/s41467-022-29531-x

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