期刊
ACS APPLIED MATERIALS & INTERFACES
卷 12, 期 32, 页码 36320-36328出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c08428
关键词
in situ TEM; transition-metal chalcogenide; lithium-ion migration; Li/V antisite; topotactic growth of Li2S
资金
- Key-Area Research and Development Program of GuangDong Province [2018B010109009]
- National Natural Science Foundation of China [51672007, 11974023, 51575135, U1537206]
- National Basic Research Program of China [2016YFA0300804, 2016YFA0300903]
- Fundamental Research Funds for the Central Universities, China [ZYGX2019Z008]
- Natural Science Foundation of Heilongjiang Province of China [YQ2019E023]
- 2011 Program Peking-Tsinghua-IOP Collaborative Innovation Center of Quantum Matter
Two-dimensional transition-metal dichalcogenides hold great potential in rechargeable lithium-ion batteries. Their electrochemical properties are closely related to the structural evolutions during lithium-ion migration. Understanding these migration/reaction mechanisms is important to help improve battery performance. Herein, we report the real-time and atomic-scale observation of phase transitions during the lithiation and delithiation for V5S8 via in situ electron diffraction and high-resolution transmission electron microscopy techniques. We find that the phase transformation proceeds via a sequence of order to antisite disorder intercalation and topotactic-based conversion reaction. During the intercalation reaction, the lithium ion destroys the orderings of the interstitial V with the formation of Li/V antisite. Such a reaction is found to be reversible, i.e., the extraction of lithium from LixV5S8 leads to the recovery of V orderings. The conversion reaction involves heterogeneous nucleation of Li2S with 3 -20 nm nanodomains, which maintain the crystallographic integrity with LixV5S8. These findings elucidate the complex interactions between the lithium ion and host V5S8 during ionic migration in solids, which should be helpful in understanding the relationship between phase transformation kinetics and battery performance.
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