期刊
NATURE NANOTECHNOLOGY
卷 7, 期 11, 页码 749-756出版社
NATURE PORTFOLIO
DOI: 10.1038/NNANO.2012.170
关键词
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资金
- Laboratory Directed Research and Development (LDRD) project at Sandia National Laboratories (SNL)
- Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center (EFRC)
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DESC0001160]
- US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
- NSF [CMMI-0758554, 1100205, DMR-1008104, DMR-1120901, CMMI-0900692]
- AFOSR [FA9550-08-1-0325]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1120901] Funding Source: National Science Foundation
- Div Of Civil, Mechanical, & Manufact Inn
- Directorate For Engineering [1100205] Funding Source: National Science Foundation
In lithium-ion batteries, the electrochemical reaction between the electrodes and lithium is a critical process that controls the capacity, cyclability and reliability of the battery. Despite intensive study, the atomistic mechanism of the electrochemical reactions occurring in these solid-state electrodes remains unclear. Here, we show that in situ transmission electron microscopy can be used to study the dynamic lithiation process of single-crystal silicon with atomic resolution. We observe a sharp interface (similar to 1 nm thick) between the crystalline silicon and an amorphous LixSi alloy. The lithiation kinetics are controlled by the migration of the interface, which occurs through a ledge mechanism involving the lateral movement of ledges on the close-packed {111} atomic planes. Such ledge flow processes produce the amorphous LixSi alloy through layer-by-layer peeling of the {111} atomic facets, resulting in the orientation-dependent mobility of the interfaces.
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