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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

Author

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  • Hyewoo Noh

    (Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
    Department of Chemical and Biological Engineering, Korea University, Seoul 02841, Republic of Korea
    These authors contributed equally to this work.)

  • Daeil Kim

    (Korea Institute of Energy Research, Daejeon 34129, Republic of Korea
    These authors contributed equally to this work.)

  • 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)

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.

Suggested Citation

  • Hyewoo Noh & Daeil Kim & Wooyoung Lee & Boyun Jang & Jeong Sook Ha & Ji Haeng Yu, 2023. "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," Energies, MDPI, vol. 16(23), pages 1-19, November.
    • Handle: RePEc:gam:jeners:v:16:y:2023:i:23:p:7695-:d:1284819
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    References listed on IDEAS

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    1. Jürgen Janek & Wolfgang G. Zeier, 2023. "Challenges in speeding up solid-state battery development," Nature Energy, Nature, vol. 8(3), pages 230-240, March.
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