Structural and Chemical Compatibilities of Li1−xNi0.5Co0.2Mn0.3O2 Cathode Material with Garnet-Type Solid Electrolyte for All-Solid-State Batteries

Seokjae Hong, Seok Hyun Song, Moses Cho, Seulgi Kim, Seung Ho Yu, Dongju Lee, Hyungsub Kim

Research output: Contribution to journalArticlepeer-review

9 Citations (Scopus)

Abstract

All-solid-state batteries (ASSBs) based on ceramic materials are considered a key technology for automobiles and energy storage systems owing to their high safety and stability. However, contact issues between the electrode and solid-electrolyte materials and undesired chemical reaction occurring at interfaces have hindered their development. Herein, the chemical compatibility and structural stability of composite mixtures of the layered cathode materials Li1−xNi0.5Co0.2Mn0.3O2 (NCM523) with the garnet-type solid electrolyte Li6.25Ga0.25La3Zr2O12 (LLZO-Ga) during high-temperature co-sintering under various gas flowing conditions are investigated. In situ high-temperature X-ray diffraction analysis of the composite materials reveals that Li diffusion from LLZO-Ga to NCM523 occurs at high temperature under synthetic air atmosphere, resulting in the decomposition of LLZO-Ga into La2Zr2O7 and the recovery of charged NCM523 to the as-prepared state. The structural stability of the composite mixture at high temperature is further investigated under N2 atmosphere, revealing that Li diffuses toward the opposite direction and involves the phase transition of LLZO-Ga from a cubic to tetragonal structure and the reduction of the NCM523 cathode to Ni metal. These findings provide insight into the structural stability of layered cathode and garnet-type solid-electrolyte composite materials and the design of stable interfaces between them via co-sintering for ASSBs.

Original languageEnglish
Article number2103306
JournalSmall
Volume17
Issue number46
DOIs
Publication statusPublished - 2021 Nov 18

Bibliographical note

Funding Information:
This work was supported by the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT of Korea (grant no. NRF‐2017M2A2A6A05017652 and NRF‐2017M1A2A2044484). This work was also supported by the internal R&D program at KAERI funded by the Ministry of Science and ICT of Korea (524210‐21).

Publisher Copyright:
© 2021 Wiley-VCH GmbH.

Keywords

  • all-solid-state batteries
  • chemical compatibility
  • interphase reaction
  • structural stability

ASJC Scopus subject areas

  • Biotechnology
  • Biomaterials
  • General Chemistry
  • General Materials Science

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