Disorder-driven sintering-free garnet-type solid electrolytes

Giyun Kwon (), Hyeokjo Gwon (), Youngjoon Bae, Changhoon Jung, Dong-Su Ko, Min Gyu Kim, Kyungho Yoon, Gabin Yoon, Sewon Kim, In-Sun Jung, Sangjun Lee, Taehee Kim, Ju-Sik Kim, Tae Young Kim and Yong Su Kim
Additional contact information
Giyun Kwon: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Hyeokjo Gwon: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Youngjoon Bae: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Changhoon Jung: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Dong-Su Ko: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Min Gyu Kim: Pohang University of Science and Technology
Kyungho Yoon: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Gabin Yoon: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Sewon Kim: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
In-Sun Jung: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Sangjun Lee: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Taehee Kim: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Ju-Sik Kim: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Tae Young Kim: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.
Yong Su Kim: Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co. Ltd.

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Oxide ceramic electrolytes for realization of high-energy lithium metal batteries typically require high-temperature processes to achieve the desired phase formation and inter-particle sintering. However, such high-temperature processing can lead to compositional changes or mechanical deformation, compromising material reliability. Here, we introduce a disorder-driven, sintering-free approach to synthesize garnet-type solid electrolyte via the creation of an amorphous matrix followed by a single-step mild heat-treatment. The softened mechanical property (yield pressure, Py = 359.8 MPa) of disordered base materials enables the facile formation of a dense amorphous matrix and the preserving of inter-particle connectivity during crystallization. The formation of the cubic-phase garnet is triggered at a lowered temperature of 350 °C, achieving a Li+ ionic conductivity of 1.8 × 10–4 S/cm at 25 °C through a single-step mild heat treatment at 500 °C. The disorder-driven garnet solid electrolyte exhibits electrochemical performance comparable to conventional garnet solid electrolyte sintered at >1100 °C. These findings will promote the fabrication of uniform, thin, and wide solid electrolyte membranes, which is a significant hurdle in the commercialization of oxide-based lithium metal batteries, and demonstrate the untapped capabilities of garnet-type oxide solid electrolytes.

Date: 2025
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DOI: 10.1038/s41467-025-58108-7

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