A locally solvent-tethered polymer electrolyte for long-life lithium metal batteries

Yanfei Zhu, Zhoujie Lao, Mengtian Zhang, Tingzheng Hou (), Xiao Xiao, Zhihong Piao, Gongxun Lu, Zhiyuan Han, Runhua Gao, Lu Nie, Xinru Wu, Yanze Song, Chaoyuan Ji, Jian Wang and Guangmin Zhou ()
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Yanfei Zhu: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Zhoujie Lao: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Mengtian Zhang: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Tingzheng Hou: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Xiao Xiao: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Zhihong Piao: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Gongxun Lu: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Zhiyuan Han: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Runhua Gao: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Lu Nie: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Xinru Wu: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Yanze Song: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Chaoyuan Ji: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School
Jian Wang: Canadian Light Source
Guangmin Zhou: Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Solid polymer electrolytes exhibit enhanced Li+ conductivity when plasticized with highly dielectric solvents such as N,N-dimethylformamide (DMF). However, the application of DMF-containing electrolytes in solid-state batteries is hindered by poor cycle life caused by continuous DMF degradation at the anode surface and the resulting unstable solid-electrolyte interphase. Here we report a composite polymer electrolyte with a rationally designed Hofmann-DMF coordination complex to address this issue. DMF is engineered on Hofmann frameworks as tethered ligands to construct a locally DMF-rich interface which promotes Li+ conduction through a ligand-assisted transport mechanism. A high ionic conductivity of 6.5 × 10−4 S cm−1 is achieved at room temperature. We demonstrate that the composite electrolyte effectively reduces the free shuttling and subsequent decomposition of DMF. The locally solvent-tethered electrolyte cycles stably for over 6000 h at 0.1 mA cm−2 in Li | |Li symmetric cell. When paired with sulfurized polyacrylonitrile cathodes, the full cell exhibits a prolonged cycle life of 1000 cycles at 1 C. This work will facilitate the development of practical polymer-based electrolytes with high ionic conductivity and long cycle life.

Date: 2024
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DOI: 10.1038/s41467-024-48078-7

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