Investigating the Interface of Li{N(SO<sub>2</sub>F)<sub>2</sub>}(NCCH<sub>2</sub>CH<sub>2</sub>CN)<sub>2</sub> Molecular Crystal Electrolytes for 5 V Class Solid-State Batteries

Molecular crystals composed of lithium bis(fluorosulfonyl)amide (LiFSA) and succinonitrile (SN), hereafter referred to as Li(FSA)(SN)<sub>2</sub>, are a promising solid electrolyte. To realize a wider application of molecular crystal solid electrolytes, it is critical to investigate the interface of Li(FSA)(SN)<sub>2</sub> and 5 V-class positive electrodes. Here, we studied the interface of Li(FSA)(SN)<sub>2</sub> with 5 V-class LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> (LNMO) positive electrodes utilizing modeled thin-film batteries. The Li(FSA)(SN)<sub>2</sub>|LNMO interfaces degrade, leading to an increase in interface resistance and capacity loss. By inserting an amorphous Li<sub>3</sub>PO<sub>4</sub> layer into the Li(FSA)(SN)<sub>2</sub>|LNMO interface, the low interface resistance remains, and no interphase layer is observed. The discharge capacity remains at 96% after 100 charge and discharge cycles. This study demonstrated the feasibility of operating Li(FSA)(SN)<sub>2</sub> in a 5 V-class solid-state battery revealing the potential of molecular crystal solid electrolytes in high-energy-density batteries.

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Publication Details

Journal
ACS Applied Materials & Interfaces
Published
2025-03-28
DOI
https://doi.org/10.1021/acsami.4c22076
Citations
1
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
0.73

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article

Investigating the Interface of Li{N(SO2F)2}(NCCH2CH2CN)2 Molecular Crystal Electrolytes for 5 V Class Solid-State Batteries

Ryota Shimizu, Ruijie Zheng, Mana Ogawa, Kazunori Nishio, Shigeru Kobayashi, Yoshitaka Tateyama, Ryo Nakayama, Makoto Moriya, Taro Hitosugi, Yuki Watanabe, Jun Deng, H. Katsuragawa
article en
1 citations

Abstract

Molecular crystals composed of lithium bis(fluorosulfonyl)amide (LiFSA) and succinonitrile (SN), hereafter referred to as Li(FSA)(SN)<sub>2</sub>, are a promising solid electrolyte. To realize a wider application of molecular crystal solid electrolytes, it is critical to investigate the interface of Li(FSA)(SN)<sub>2</sub> and 5 V-class positive electrodes. Here, we studied the interface of Li(FSA)(SN)<sub>2</sub> with 5 V-class LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> (LNMO) positive electrodes utilizing modeled thin-film batteries. The Li(FSA)(SN)<sub>2</sub>|LNMO interfaces degrade, leading to an increase in interface resistance and capacity loss. By inserting an amorphous Li<sub>3</sub>PO<sub>4</sub> layer into the Li(FSA)(SN)<sub>2</sub>|LNMO interface, the low interface resistance remains, and no interphase layer is observed. The discharge capacity remains at 96% after 100 charge and discharge cycles. This study demonstrated the feasibility of operating Li(FSA)(SN)<sub>2</sub> in a 5 V-class solid-state battery revealing the potential of molecular crystal solid electrolytes in high-energy-density batteries.

ACS Applied Materials & InterfacesVol. 17(14)
Shizuoka University (JP), National Institute for Materials Science (JP), Shanghai Institute for Science of Science (CN), Life Science Institute (JP), Institute of Science Tokyo (JP), The University of Tokyo (JP)
Ministry of Education, Culture, Sports, Science and Technology, Japan Society for the Promotion of Science, Core Research for Evolutional Science and Technology, JST-Mirai Program
Openalex Percentile: Top 30%
Advancements in Battery Materials
0.73
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