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Vol. 15 (2023)

Elucidating Ion Transport Phenomena in Sulfide/Polymer Composite Electrolytes for Practical Solid-State Batteries

https://doi.org/10.1007/s40820-023-01139-w
Kyeong‑Seok Oh
Department of Chemical and Biomolecular Engineering, Yonsei University, 50 Yonsei‑ro, Seodaemun‑gu, Seoul 03722, Republic of Korea
Ji Eun Lee
School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST‑gil, Eonyang‑eup, Ulju‑gun, Ulsan 44919, Republic of Korea
Yong‑Hyeok Lee
Department of Chemical and Biomolecular Engineering, Yonsei University, 50 Yonsei‑ro, Seodaemun‑gu, Seoul 03722, Republic of Korea
Yi‑Su Jeong
School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST‑gil, Eonyang‑eup, Ulju‑gun, Ulsan 44919, Republic of Korea
Imanuel Kristanto
Department of Chemical and Biological Engineering, Korea University, 145 Anam‑ro, Seongbuk‑gu, Seoul 02841, Republic of Korea
Hong‑Seok Min
Hyundai Motor Company, 150, Hyundaiyeonguso‑ro, Namyang‑eup, Hwaseong‑si, Gyeonggi‑do 18280, Republic of Korea
Sang‑Mo Kim
Hyundai Motor Company, 150, Hyundaiyeonguso‑ro, Namyang‑eup, Hwaseong‑si, Gyeonggi‑do 18280, Republic of Korea
Young Jun Hong
Hyundai Motor Company, 150, Hyundaiyeonguso‑ro, Namyang‑eup, Hwaseong‑si, Gyeonggi‑do 18280, Republic of Korea
Sang Kyu Kwak
Department of Chemical and Biological Engineering, Korea University, 145 Anam‑ro, Seongbuk‑gu, Seoul 02841, Republic of Korea
Sang‑Young Lee
Department of Chemical and Biomolecular Engineering, Yonsei University, 50 Yonsei‑ro, Seodaemun‑gu, Seoul 03722, Republic of Korea

Corresponding Author: Sang‑Young Lee

syleek@yonsei.ac.kr

Nano-Micro Letters, Vol. 15 (2023), Article Number: 179

Abstract

Despite the enormous interest in inorganic/polymer composite solid-state electrolytes (CSEs) for solid-state batteries (SSBs), the underlying ion transport phenomena in CSEs have not yet been elucidated. Here, we address this issue by formulating a mechanistic understanding of bi-percolating ion channels formation and ion conduction across inorganic-polymer electrolyte interfaces in CSEs. A model CSE is composed of argyrodite-type Li6PS5Cl (LPSCl) and gel polymer electrolyte (GPE, including Li+-glyme complex as an ion-conducting medium). The percolation threshold of the LPSCl phase in the CSE strongly depends on the elasticity of the GPE phase. Additionally, manipulating the solvation/desolvation behavior of the Li+-glyme complex in the GPE facilitates ion conduction across the LPSCl-GPE interface. The resulting scalable CSE (area = 8 × 6 (cm × cm), thickness ~ 40 μm) can be assembled with a high-mass-loading LiNi0.7Co0.15Mn0.15O2 cathode (areal-mass-loading = 39 mg cm–2) and a graphite anode (negative (N)/positive (P) capacity ratio = 1.1) in order to fabricate an SSB full cell with bi-cell configuration. Under this constrained cell condition, the SSB full cell exhibits high volumetric energy density (480 Wh Lcell−1) and stable cyclability at 25 °C, far exceeding the values reported by previous CSE-based SSBs.


Highlights:
1 Mechanistic understanding of ion transport phenomena in composite solid-state electrolytes (CSEs) for practical solid-state batteries is conducted.
2 Percolation threshold formation of the inorganic (LPSCl) phase in the CSEs depends on elasticity of the gel polymer electrolyte (GPE) phase.
3 Manipulating the solvation/desolvation behavior of the GPE phase facilitates ion conduction across the LPSCl-GPE interfaces.

Keywords

Solid-state batteries Composite solid-state electrolytes Ion transport phenomena Bi-percolating ion channels Interfacial resistance
Oh, Kyeong‑Seok, Ji Eun Lee, Yong‑Hyeok Lee, Yi‑Su Jeong, Imanuel Kristanto, Hong‑Seok Min, Sang‑Mo Kim, Young Jun Hong, Sang Kyu Kwak, and Sang‑Young Lee. 2023. “Elucidating Ion Transport Phenomena in Sulfide/Polymer Composite Electrolytes for Practical Solid-State Batteries”. Nano-Micro Letters 15 (July):179. https://doi.org/10.1007/s40820-023-01139-w.
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