Dense Sphene-type Solid Electrolyte Through Rapid Sintering for Solid-state Lithium Metal Battery

doi:10.1007/s40242-020-0114-2

高等学校化学研究 ›› 2020, Vol. 36 ›› Issue (3): 439-446.doi: 10.1007/s40242-020-0114-2

Dense Sphene-type Solid Electrolyte Through Rapid Sintering for Solid-state Lithium Metal Battery

WANG Yongtao, GUO Xianwei, LIN Zhiyuan, YANG Yubo, WU Lingqiao, LIU Huan, YU Haijun

College of Materials Science & Engineering, Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing 100124, P. R. China

收稿日期:2020-04-15 修回日期:2020-05-13 出版日期:2020-06-01 发布日期:2020-05-30
通讯作者: GUO Xianwei, YU Haijun E-mail:hj-yu@bjut.edu.cn;xwguo@bjut.edu.cn
基金资助:
Supported by the Natural Science Foundation of Beijing, China(Nos.KZ201910005002, JQ19003, L182009), the National Natural Science Foundation of China(Nos.51622202, 21974007), the National Key R&D Program of China(No.2018YFB-0104300), and the Project of Youth Talent Plan of Beijing Municipal Education Commission, China(No.CIT&TCD201804013).

Dense Sphene-type Solid Electrolyte Through Rapid Sintering for Solid-state Lithium Metal Battery

WANG Yongtao, GUO Xianwei, LIN Zhiyuan, YANG Yubo, WU Lingqiao, LIU Huan, YU Haijun

College of Materials Science & Engineering, Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing 100124, P. R. China

Received:2020-04-15 Revised:2020-05-13 Online:2020-06-01 Published:2020-05-30
Contact: GUO Xianwei, YU Haijun E-mail:hj-yu@bjut.edu.cn;xwguo@bjut.edu.cn
Supported by:
Supported by the Natural Science Foundation of Beijing, China(Nos.KZ201910005002, JQ19003, L182009), the National Natural Science Foundation of China(Nos.51622202, 21974007), the National Key R&D Program of China(No.2018YFB-0104300), and the Project of Youth Talent Plan of Beijing Municipal Education Commission, China(No.CIT&TCD201804013).

摘要/Abstract

摘要： The sphene-type solid electrolyte with high ionic conductivity has been designed for solid-state lithium metal battery. However, the practical applications of solid electrolytes are still suffered by the low relative density and long sintering time of tens of hours with large energy consumption. Here, we introduced the spark plasma sintering technology for fabricating the sphene-type Li_1.125Ta_0.875Zr_0.125SiO₅ solid electrolyte. The dense electrolyte pellet with high relative density of ca. 97.4% and ionic conductivity of ca. 1.44×10^-5 S/cm at 30℃ can be obtained by spark plasma sintering process within the extremely short time of only ca. 0.1 h. Also the solid electrolyte provides stable electrochemical window of ca. 6.0 V(vs. Li⁺/Li) and high electrochemical interface stability toward Li metal anode. With the enhanced interfacial contacts between electrodes and electrolyte pellet by the in-situ formed polymer electrolyte, the solid-state lithium metal battery with LiFePO₄ cathode can deliver the initial discharge capacity of ca. 154 mA·h/g at 0.1 C and the reversible capacity of ca. 132 mA·h/g after 70 cycles with high Coulombic efficiency of 99.5% at 55℃. Therefore, this study demonstrates a rapid and energy efficient sintering strategy for fabricating the solid electrolyte with dense structure and high ionic conductivity that can be practically applied in solid-state lithium metal batteries with high energy densities and safeties.

关键词: Solid-state lithium metal battery, Sphene-type solid electrolyte, Spark plasma sintering, Dense structure, Ionic conductivity

Abstract: The sphene-type solid electrolyte with high ionic conductivity has been designed for solid-state lithium metal battery. However, the practical applications of solid electrolytes are still suffered by the low relative density and long sintering time of tens of hours with large energy consumption. Here, we introduced the spark plasma sintering technology for fabricating the sphene-type Li_1.125Ta_0.875Zr_0.125SiO₅ solid electrolyte. The dense electrolyte pellet with high relative density of ca. 97.4% and ionic conductivity of ca. 1.44×10^-5 S/cm at 30℃ can be obtained by spark plasma sintering process within the extremely short time of only ca. 0.1 h. Also the solid electrolyte provides stable electrochemical window of ca. 6.0 V(vs. Li⁺/Li) and high electrochemical interface stability toward Li metal anode. With the enhanced interfacial contacts between electrodes and electrolyte pellet by the in-situ formed polymer electrolyte, the solid-state lithium metal battery with LiFePO₄ cathode can deliver the initial discharge capacity of ca. 154 mA·h/g at 0.1 C and the reversible capacity of ca. 132 mA·h/g after 70 cycles with high Coulombic efficiency of 99.5% at 55℃. Therefore, this study demonstrates a rapid and energy efficient sintering strategy for fabricating the solid electrolyte with dense structure and high ionic conductivity that can be practically applied in solid-state lithium metal batteries with high energy densities and safeties.

Key words: Solid-state lithium metal battery, Sphene-type solid electrolyte, Spark plasma sintering, Dense structure, Ionic conductivity

WANG Yongtao, GUO Xianwei, LIN Zhiyuan, YANG Yubo, WU Lingqiao, LIU Huan, YU Haijun. Dense Sphene-type Solid Electrolyte Through Rapid Sintering for Solid-state Lithium Metal Battery[J]. 高等学校化学研究, 2020, 36(3): 439-446.

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Dense Sphene-type Solid Electrolyte Through Rapid Sintering for Solid-state Lithium Metal Battery

Dense Sphene-type Solid Electrolyte Through Rapid Sintering for Solid-state Lithium Metal Battery

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