Investigating theInterface of Li{N(SO<sub>2</sub>F)<sub>2</sub>}(NCCH<sub>2</sub>CH<sub>2</sub>CN)<sub>2</sub> MolecularCrystal 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.

Publication Details

Journal
Figshare
Published
2025-03-28
DOI
https://doi.org/10.1021/acsami.4c22076.s001
Primary Topic
Advanced Battery Materials and Technologies
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Investigating theInterface of Li{N(SO2F)2}(NCCH2CH2CN)2 MolecularCrystal Electrolytes for 5 V Class Solid-State Batteries

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Advanced Battery Materials and Technologies
article

Investigating theInterface of Li{N(SO2F)2}(NCCH2CH2CN)2 MolecularCrystal Electrolytes for 5 V Class Solid-State Batteries

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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.

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Investigating theInterface of Li{N(SO<sub>2</sub>F)<sub>2</sub>}(NCCH<sub>2</sub>CH<sub>2</sub>CN)<sub>2</sub> MolecularCrystal Electrolytes for 5 V Class Solid-State Batteries · Figshare (2025) | TGRS Research Map | TGRS