期刊
NANO LETTERS
卷 16, 期 9, 页码 5582-5588出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b02136
关键词
Lithitim ion battery; in situ TEM; first-principles calculation; intermediate phase; electrochemistry dynamics
类别
资金
- National Natural Science Foundation of China [51502007, 51502032, 51522201]
- National Basic Research Program of China [2016YFA0300903]
- National Program for Thousand Young Talents of China
- Peking-Tsinghua-IOP Collaborative Innovation Center of Quantum Matter
- National Science Foundation [ACT-1053575]
In the rechargeable lithium ion batteries, the rate capability and energy efficiency are largely governed by the lithium ion transport dynamics and phase transition pathways in electrodes. Real-time and atomic-scale tracking of fully reversible lithium insertion and extraction processes in electrodes, which would ultimately lead to mechanistic understanding of how the electrodes function and why they fail, is highly desirable but very challenging. Here, we track lithium insertion and extraction in the van der Waals interactions dominated SnS2 by in situ high-resolution TEM method. We find that the lithium insertion occurs via a fast two-phase reaction to form expanded and defective LiSnS2, while the lithium extraction initially involves heterogeneous nucleation of intermediate superstructure Li0.5SnS2 domains with a 14 nm size. Density functional theory calculations indicate that the Li0.5SnS2 is kinetically favored and structurally stable. The asymmetric reaction pathways may supply enlightening insights into the mechanistic understanding of the underlying electrochemistry in the layered electrode materials and also suggest possible alternatives to the accepted explanation of the origins of voltage hysteresis in the intercalation electrode materials.
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