Journal
NANO LETTERS
Volume 21, Issue 16, Pages 6859-6866Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01910
Keywords
solid-state batteries; Li dendrite; Li propagation; deposition stress; CNT fracture
Categories
Funding
- National Natural Science Foundation of China [52022088, 51971245, 51772262, 21406191, U20A20336, 21935009]
- Beijing Natural Science Foundation [2202046]
- Fok Ying-Tong Education Foundation of China [171064]
- Natural Science Foundation of Hebei Province [B2020203037, B2018203297]
- Hunan Innovation Team [2018RS3091]
- Assistant Secretary for Energy, Vehicles Technology Office, of the U.S. Department of Energy [DEAC02-05CH11231]
- Institute for Basic Science of South Korea [IBS-R019-D1]
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This study visualizes the lithium deposition dynamics in carbon nanotubes to mimic the solid-state electrolyte crack behavior, revealing the mechanism of lithium deposition in confined spaces. The deposited lithium propagates as a creeping solid in the CNTs, providing an effective pathway for stress relaxation. The research suggests that interfacial lithiophilicity critically governs lithium deposition dynamics and stress relaxation.
The increasing demand for safe and dense energy storage has shifted research focus from liquid electrolyte-based Li-ion batteries toward solid-state batteries (SSBs). However, the application of SSBs is impeded by uncontrollable Li dendrite growth and short circuiting, the mechanism of which remains elusive. Herein, we conceptualize a scheme to visualize Li deposition in the confined space inside carbon nanotubes (CNTs) to mimic Li deposition dynamics inside solid electrolyte (SE) cracks, where the high-strength CNT walls mimic the mechanically strong SEs. We observed that the deposited Li propagates as a creeping solid in the CNTs, presenting an effective pathway for stress relaxation. When the stress-relaxation pathway is blocked, the Li deposition-induced stress reaches the gigapascal level and causes CNT fracture. Mechanics analysis suggests that interfacial lithiophilicity critically governs Li deposition dynamics and stress relaxation. Our study offers critical strategies for suppressing Li dendritic growth and constructing high-energy-density, electrochemically and mechanically robust SSBs.
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