Lithium dendrite (filaments) propagation in solid electrolytes (SEs) leading to short circuits is one of the biggest obstacles to the application of all-solid-state lithium metal batteries. Due to the lack of operando techniques that can provide high resolution, the insufficient knowledge of the lithium dendrite growth inside SEs makes it difficult to suppress the dendrite growth. To reveal the mechanism of the Li filament growth in SEs, we achieved real-time monitoring of the nanoscale Li filament growth by operando small-angle neutron scattering (SANS) in representative Li6.5La3Zr1.5Nb0.5O12 SEs. On continuous plating, the Li filament growth is not simply an accumulation of Li, but there is a dynamic evolution due to the competition between the Li filament growth and self-healing. With the aid of simulations and experiments, this dynamic competition was demonstrated to be highly dependent on temperature variation. The enhanced self-healing ability of Li at elevated temperatures plays a positive role in suppressing the Li filament growth. The heat therapy improved the cell's cycle life, which provided insight into suppressing the Li filament growth. Operando SANS with high Li sensitivity provides a platform for investigating Li filaments in SEs.
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Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering
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17 October 2022
Research Article|
October 20 2022
Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering
Special Collection:
New Technologies and New Applications of Advanced Batteries
Jinghao Yang;
Jinghao Yang
(Conceptualization, Data curation, Formal analysis, Investigation, Methodology, Visualization, Writing – original draft)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
2
Key Laboratory for Neutron Physics of Chinese Academy of Engineering Physics, Institute of Nuclear Physics and Chemistry
, Mianyang 621999, China
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Fangjie Mo;
Fangjie Mo
(Conceptualization, Formal analysis, Methodology)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
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Jiaming Hu;
Jiaming Hu
(Data curation, Formal analysis, Methodology, Software, Visualization)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
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Shuyang Li;
Shuyang Li
(Data curation, Investigation)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
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Lizhao Huang;
Lizhao Huang
(Conceptualization, Formal analysis, Methodology, Software)
2
Key Laboratory for Neutron Physics of Chinese Academy of Engineering Physics, Institute of Nuclear Physics and Chemistry
, Mianyang 621999, China
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Fang Fang;
Fang Fang
(Funding acquisition, Project administration, Resources)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
3
Yiwu Research Institute of Fudan University, Yiwu City
, Zhejiang 322000, People's Republic of China
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Dalin Sun;
Dalin Sun
(Funding acquisition, Resources, Supervision)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
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Guangai Sun;
Guangai Sun
(Project administration, Resources, Supervision)
2
Key Laboratory for Neutron Physics of Chinese Academy of Engineering Physics, Institute of Nuclear Physics and Chemistry
, Mianyang 621999, China
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Fei Wang
;
Fei Wang
a)
(Formal analysis, Funding acquisition, Project administration, Validation, Writing – review & editing)
1
Department of Materials Science, Fudan University
, Shanghai 200433, China
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Note: This paper is part of the APL Special Collection on New Technologies and New Applications of Advanced Batteries.
Appl. Phys. Lett. 121, 163901 (2022)
Article history
Received:
July 17 2022
Accepted:
September 27 2022
Citation
Jinghao Yang, Fangjie Mo, Jiaming Hu, Shuyang Li, Lizhao Huang, Fang Fang, Dalin Sun, Guangai Sun, Fei Wang, Yun Song; Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering. Appl. Phys. Lett. 17 October 2022; 121 (16): 163901. https://doi.org/10.1063/5.0110830
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