Garnet-rich composite solid electrolytes for dendrite-free, high-rate, solid-state lithium-metal batteries

Yan, Chaoyi; Zhu, Pei; Jia, Hao; Du, Zhuang; Zhu, Jiadeng; Orenstein, Raphael; Cheng, Hui; Wu, Nianqiang; Dirican, Mahmut; Zhang, Xiangwu

doi:10.1016/j.ensm.2019.11.018

Garnet-rich composite solid electrolytes for dendrite-free, high-rate, solid-state lithium-metal batteries

Journal Article · Wed Nov 20 23:00:00 EST 2019 · Energy Storage Materials

DOI:https://doi.org/10.1016/j.ensm.2019.11.018· OSTI ID:1799379

^[1]; Zhu, Pei ^[2]; Jia, Hao ^[2]; Du, Zhuang ^[2]; ^[2]; Orenstein, Raphael ^[2]; Cheng, Hui ^[2]; ^[3]; ^[2]; ^[2]

North Carolina State Univ., Raleigh, NC (United States); OSTI
North Carolina State Univ., Raleigh, NC (United States)
West Virginia Univ., Morgantown, WV (United States)

Composite solid electrolytes (CSEs), which are composed of inorganic fillers and organic polymers, show improved safety and suppressed lithium dendrite growth in Li-metal batteries, as compared to flammable liquid electrolytes. However, the performance of current CSEs is limited by the agglomeration effect, with low content of inorganic Li⁺-conducting fillers and ineffective Li⁺ transport between the inorganic fillers and the polymer matrix. To address these challenges, a new type of CSE composed of silane-modified Li_6.28La₃Al_0.24Zr₂O₁₂ (s@LLAZO) nanofibers and poly(ethylene glycol) diacrylate (PEGDA) is developed. Employment of the silane coupling agent, 3-(trimethoxysilyl)propyl methacrylate, enables the incorporation of a high content of LLAZO nanofibers (up to 70 wt%) with the polymer matrix and results in a well-percolated, three-dimensional LLAZO network fully embedded in the PEGDA matrix. Consequently, the silane coupling agent successfully eliminates the agglomeration effect, which ensures higher ionic conductivity, larger lithium transference number, wider electrochemical stability window, and better cycling stability for s@LLZAO-PEGDA CSEs. Excellent cycling stability and extraordinarily high rate capability (up to 10C) are demonstrated in the all-solid-state Li-metal batteries with LiFePO₄ and high-voltage Li[Ni_1/3Mn_1/3Co_1/3]O₂ cathodes at ambient temperature. This novel design of CSEs with s@LLAZO nanofibers paves the way for a new generation of improved functioning all-solid-state Li-metal batteries.

View Accepted Manuscript (DOE)

Research Organization:: West Virginia Univ., Morgantown, WV (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: EE0007806

OSTI ID:: 1799379

Alternate ID(s):: OSTI ID: 1601892

Journal Information:: Energy Storage Materials, Journal Name: Energy Storage Materials Vol. 26; ISSN 2405-8297

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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all-solid-state batteries
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