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- Title
Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li<sub>6.1</sub>Ga<sub>0.3</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>.
- Authors
Lee, Rae-Hyun; Kang, Chea-Yun; Lee, Jong-Kyu; Jin, Bong-Soo; Kim, Kyong-Nam; Kim, Hyun-Soo; Yoon, Jung-Rag; Lee, Seung-Hwan
- Abstract
Garnet-type Li6.1Ga0.3La3Zr2O12 (LGLZO) exhibits high ionic conductivity and extremely low electronic conductivity. The electrochemical properties strongly depend on the characteristics of the grain boundaries and pores in the oxide–ceramic electrolyte. Currently, the main issue of LGLZO is its large grain boundary resistance due to high-temperature sintering. Herein, we propose an effective method for reinforcing the chemical and structural characteristics of the grain boundaries using a Li2O-B2O3-Al2O3 (LBA) sintering aid. In this study, the LBA sintering aid is critical because it fills grain boundaries and void spaces. As a result, LGLZO solid-state electrolytes with sintering aids significantly enhance the ionic conductivity and reduce the activation energy, especially in the grain boundary region. Another crucial issue is the formation of Li dendrites in LGLZO. Since dendritic Li propagates along the grain boundaries, the optimized LGLZO solid-state electrolyte demonstrates excellent stability against Li metals. Overall, the LGLZO electrolyte with the LBA sintering aid exhibits stable long-term cycling performance due to the well-designed grain boundaries. The addition of Li2O-B2O3-Al2O3 (LBA) sintering aid to Li6.1Ga0.3La3Zr2O12 (LGLZO) solid electrolytes enhances grain boundary characteristics and reduces porosity. This modification leads to a substantial increase in ionic conductivity and mechanical stability, while effectively preventing Li dendrite formation. The optimized LGLZO sample with LBA exhibits improved long-term cycling performance, making it a promising candidate for high-performance all-solid-state batteries. These findings underscore the critical role of grain boundary engineering in enhancing the electrochemical properties of garnet-type electrolytes.
- Subjects
GARNET; CRYSTAL grain boundaries; SOLID electrolytes; ALUMINUM-lithium alloys; IONIC conductivity; ACTIVATION energy; DENDRITES
- Publication
NPG Asia Materials, 2024, Vol 16, Issue 1, p1
- ISSN
1884-4049
- Publication type
Article
- DOI
10.1038/s41427-024-00563-7