Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries
Molecular crystal electrolytes are promising solid electrolytes owing to their ionic conductivity and mechanical flexibility. However, solid-state batteries using these electrolytes suffer from the large resistance at the interfaces with positive electrodes. Herein, we fabricate a battery using Li{N...
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| Format: | Article |
| Language: | English |
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AIP Publishing LLC
2025-01-01
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| Series: | APL Materials |
| Online Access: | http://dx.doi.org/10.1063/5.0241289 |
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| author | Yuki Watanabe Shigeru Kobayashi Zheng Ruijie Deng Jun Kenjiro Tanaka Kazunori Nishio Ryo Nakayama Ryota Shimizu Makoto Moriya Taro Hitosugi |
| author_facet | Yuki Watanabe Shigeru Kobayashi Zheng Ruijie Deng Jun Kenjiro Tanaka Kazunori Nishio Ryo Nakayama Ryota Shimizu Makoto Moriya Taro Hitosugi |
| author_sort | Yuki Watanabe |
| collection | DOAJ |
| description | Molecular crystal electrolytes are promising solid electrolytes owing to their ionic conductivity and mechanical flexibility. However, solid-state batteries using these electrolytes suffer from the large resistance at the interfaces with positive electrodes. Herein, we fabricate a battery using Li{N(SO2F)2}(NCCH2CH2CN)2, referred to as Li(FSA)(SN)2, a molecular-crystal electrolyte, and demonstrate the stable thin-film battery cycling. The novel fabrication method forms electrochemically stable interfaces, allowing the thin-film batteries to cycle at a current density of up to 500 μA cm−2 in the voltage range of 3.00–4.05 V vs Li/Li+. This current density is 500 times higher than that reported previously. Notably, the Li(FSA)(SN)2–LiCoO2 interface resistance (24 Ω cm2) is comparable to that of the interface of liquid-electrolyte and LiCoO2 in Li-ion batteries. Furthermore, inserting an amorphous Li3PO4 layer into the Li(FSA)(SN)2–LiCoO2 interface enables stable cycling up to 4.30 V vs Li/Li+, suppressing the decomposition of electrolytes. These quantitative investigations and interfacial controls pave the way for the practical applications of molecular-crystal electrolytes to solid-state batteries. |
| format | Article |
| id | doaj-art-6d30c510b5304b98a966af3caf544aa4 |
| institution | Kabale University |
| issn | 2166-532X |
| language | English |
| publishDate | 2025-01-01 |
| publisher | AIP Publishing LLC |
| record_format | Article |
| series | APL Materials |
| spelling | doaj-art-6d30c510b5304b98a966af3caf544aa42025-02-03T16:42:31ZengAIP Publishing LLCAPL Materials2166-532X2025-01-01131011122011122-710.1063/5.0241289Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteriesYuki Watanabe0Shigeru Kobayashi1Zheng Ruijie2Deng Jun3Kenjiro Tanaka4Kazunori Nishio5Ryo Nakayama6Ryota Shimizu7Makoto Moriya8Taro Hitosugi9School of Materials and Chemical Technology, Tokyo Institute of Technology, Tokyo 152-8552, JapanDepartment of Chemistry, The University of Tokyo, Tokyo 113-0033, JapanSchool of Materials and Chemical Technology, Tokyo Institute of Technology, Tokyo 152-8552, JapanSchool of Materials and Chemical Technology, Tokyo Institute of Technology, Tokyo 152-8552, JapanDepartment of Science, Graduate School of Integrated Science and Technology, Shizuoka University, Shizuoka 422-8529, JapanSchool of Materials and Chemical Technology, Tokyo Institute of Technology, Tokyo 152-8552, JapanDepartment of Chemistry, The University of Tokyo, Tokyo 113-0033, JapanDepartment of Chemistry, The University of Tokyo, Tokyo 113-0033, JapanCollege of Science, Academic Institute, Shizuoka University, Shizuoka 422-8529, JapanSchool of Materials and Chemical Technology, Tokyo Institute of Technology, Tokyo 152-8552, JapanMolecular crystal electrolytes are promising solid electrolytes owing to their ionic conductivity and mechanical flexibility. However, solid-state batteries using these electrolytes suffer from the large resistance at the interfaces with positive electrodes. Herein, we fabricate a battery using Li{N(SO2F)2}(NCCH2CH2CN)2, referred to as Li(FSA)(SN)2, a molecular-crystal electrolyte, and demonstrate the stable thin-film battery cycling. The novel fabrication method forms electrochemically stable interfaces, allowing the thin-film batteries to cycle at a current density of up to 500 μA cm−2 in the voltage range of 3.00–4.05 V vs Li/Li+. This current density is 500 times higher than that reported previously. Notably, the Li(FSA)(SN)2–LiCoO2 interface resistance (24 Ω cm2) is comparable to that of the interface of liquid-electrolyte and LiCoO2 in Li-ion batteries. Furthermore, inserting an amorphous Li3PO4 layer into the Li(FSA)(SN)2–LiCoO2 interface enables stable cycling up to 4.30 V vs Li/Li+, suppressing the decomposition of electrolytes. These quantitative investigations and interfacial controls pave the way for the practical applications of molecular-crystal electrolytes to solid-state batteries.http://dx.doi.org/10.1063/5.0241289 |
| spellingShingle | Yuki Watanabe Shigeru Kobayashi Zheng Ruijie Deng Jun Kenjiro Tanaka Kazunori Nishio Ryo Nakayama Ryota Shimizu Makoto Moriya Taro Hitosugi Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries APL Materials |
| title | Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries |
| title_full | Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries |
| title_fullStr | Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries |
| title_full_unstemmed | Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries |
| title_short | Reduced resistance at molecular-crystal electrolyte and LiCoO2 interfaces for high-performance solid-state lithium batteries |
| title_sort | reduced resistance at molecular crystal electrolyte and licoo2 interfaces for high performance solid state lithium batteries |
| url | http://dx.doi.org/10.1063/5.0241289 |
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