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journal article·2026-04Open access

Vacancy‐Suppressed Garnet Electrolytes for Durable Solid‐State Batteries

Seokjae Hong, Kwang Ho Shin, Kyoung Sun Kim, Jinhwan Kim, Jaegi Lee, Byung‐Gun Park, Won G. Hong, In Hye Kwak, Kyubin Shim, Young‐Sang Yu, Ju Young Kim, Young Hwa Jung, Min Wook Pin, Hyeon‐Jong Lee, Hojoon Kim, Dong‐Hwa Seo, Hosun Shin, Dongju Lee, Seung‐Ho Yu, Sung‐Kyun Jung, Hyungsub Kim

Advanced Science· Volume 13· Issue 21
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Source abstract

Abstract

ABSTRACT Cubic‐garnet‐type solid electrolytes (SEs) are promising candidates for all‐solid‐state batteries (ASSBs) due to their high ionic conductivity and stability against lithium metal. However, intrinsic lithium and oxygen vacancies formed during high‐temperature sintering can lead to interfacial metal reduction and phase transitions, ultimately causing short circuits. In this study, we quantified these intrinsic vacancies in Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) and proposed a strategy to achieve vacancy‐suppressed, lithium‐stuffed garnet SEs by simply tuning the lithium content in both the green pellet and bedding powder during sintering. The optimized Li‐stuffed LLZTO exhibited lithium occupancy exceeding 6.5 per formula unit (pfu) and oxygen‐vacancy concentrations below 0.02 pfu, resulting in improved chemical stability at the electrolyte–electrode interface and enhanced air stability. The garnet electrolyte demonstrated a critical current density of 1.00 mA cm −2 at 30°C and 1.75 mA cm −2 at 60°C, along with stable cycling performance over 3000 h in lithium symmetric cells and 2000 cycles in hybrid full‐cells, demonstrating 90% capacity retention. These findings highlight the pivotal role of intrinsic vacancy control in enhancing the structural and electrochemical integrity of garnet electrolytes, thereby promoting their practical application in ASSBs.
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Research context

Energy storageCeramics & glasses

OpenAlex topics: Advanced Battery Materials and Technologies · Thermal Expansion and Ionic Conductivity · Advancements in Battery Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Neutron Science Division Korea Atomic Energy Research Institute (KAERI) Yuseong‐gu Daejeon Republic of Korea

Department of Chemical and Biological Engineering Korea University Seongbuk‐gu Seoul Republic of Korea

Division of Chemical and Material Metrology‐Emerging Material Metrology Group Korea Research Institute of Standard and Science (KRISS) Yuseong‐gu Daejeon Republic of Korea

Institute For Rechargeable Battery Innovations Research Seoul National University (SNU) Seoul Republic of Korea

HANARO Utilization Division Korea Atomic Energy Research Institute (KAERI) Yuseong‐gu Daejeon Republic of Korea

Strategic Research Center for Smart Battery Korea Basic Science Institute (KBSI) Yuseong‐gu Daejeon Republic of Korea

Department of Physics Chungbuk National University Cheongju Chungbuk Republic of Korea

Smart Materials Research Section Electronics and Telecommunications Research Institute (ETRI) Yuseong‐gu Daejeon Republic of Korea

Beamline Division Pohang Accelerator Laboratory (PAL) Pohang Republic of Korea

Analysis and Assessment Group Research Institute of Industrial Science and Technology (RIST) Pohang Republic of Korea

Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology (KAIST) Daejeon Republic of Korea

Department of Applied Measurement Science University of Science and Technology (UST) Yuseong‐gu Daejeon Republic of Korea

Department of Urban, Energy, and Environmental Engineering Chungbuk National University Cheongju Chungbuk Republic of Korea

Advanced Energy Research Institute Chungbuk National University Cheongju Chungbuk Republic of Korea

Research Institute of Advanced Materials (RIAM) Seoul National University (SNU) Seoul Republic of Korea

School of Transdisciplinary Innovations Seoul National University (SNU) Seoul Republic of Korea

Department of Materials Science and Engineering Seoul National University (SNU) Seoul Republic of Korea

Funding

National Research Council of Science and Technology · National Research Foundation of Korea

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