American Chemical Society
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Lithium Deposition-Induced Fracture of Carbon Nanotubes and Its Implication to Solid-State Batteries

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journal contribution
posted on 2021-08-09, 15:44 authored by Jingzhao Chen, Chao Zhao, Dingchuan Xue, Liqiang Zhang, Tingting Yang, Congcong Du, Xuedong Zhang, Ruyue Fang, Baiyu Guo, Hongjun Ye, Hui Li, Qiushi Dai, Jun Zhao, Yanshuai Li, Stephen J. Harris, Yongfu Tang, Feng Ding, Sulin Zhang, Jianyu Huang
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.