Surface Modification of Ga-Doped-LLZO (Li 7 La 3 Zr 2 O 12 ) by the Addition of Polyacrylonitrile for the Electrochemical Stability of Composite Solid Electrolytes

Hyewoo Noh, Daeil Kim, Wooyoung Lee, Boyun Jang (), Jeong Sook Ha () and Ji Haeng Yu ()
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Hyewoo Noh: Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
Daeil Kim: Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
Wooyoung Lee: Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
Boyun Jang: Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
Jeong Sook Ha: Department of Chemical and Biological Engineering, Korea University, Seoul 02841, Republic of Korea
Ji Haeng Yu: Korea Institute of Energy Research, Daejeon 34129, Republic of Korea

Energies, 2023, vol. 16, issue 23, 1-19

Abstract: Composite solid electrolytes (CSEs), often incorporating succinonitrile (SCN), offer promi I confirm sing solutions for improving the performance of all-solid-state batteries. These electrolytes are typically made of ceramics such as Li 7 La 3 Zr 2 O 12 (LLZO) and polymers such as poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP). Garnet-applied polymer–ceramic electrolyte (g-PCE) is composed of PVDF-HFP, SCN, and LLZO. However, the interface between SCN and LLZO is reportedly unstable owing to the polymerization of SCN. This polymerization could cause two serious problems: (1) gelation during the mixing of LLZO and SCN and (2) degradation of ionic performance during charge and discharge. To prevent this catalytic reaction, polyacrylonitrile (PAN) can be added to the g-PCE (g-PPCE). PAN blocks the polymerization of SCN through a cyclization process involving La ions which occurs more rapidly than SCN polymerization. In this study, the enhanced chemical stability of the garnet-applied PAN-added polymer ceramic electrolyte (g-PPCE) was achieved by using an impregnation process which added SCN with 5 wt.% of PAN. The resulting CSE has an ionic conductivity of ~10 - ⁴ S/cm at room temperature. Coin-type cells assembled with LFP (LiFePO 4 ) and LNCM (LiNi 0 . 6 Co 0 . 2 Mn 0 . 2 O 2 ) cathodes with Li-metal anodes show specific discharge capacities of 150 and 167 mAh/g at 0.1 C, respectively, and stable cycle performance. Additionally, a pouch-type cell with a discharge capacity of 5 mAh also exhibits potential electrochemical performance.

Keywords: composite solid electrolyte; garnet oxide; polymerization; cyclization; solid-state Li-metal battery (search for similar items in EconPapers)
JEL-codes: Q Q0 Q4 Q40 Q41 Q42 Q43 Q47 Q48 Q49 (search for similar items in EconPapers)
Date: 2023
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