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Nano Lett. 2014 Sep 10;14(9):5301-7. doi: 10.1021/nl502347z. Epub 2014 Aug 28.

Lithiation-induced shuffling of atomic stacks.

Author information

1
Department of Mechanical Engineering-Engineering Mechanics, Michigan Technological University , 1400 Townsend Drive, Houghton, Michigan 49931, United States.

Abstract

In rechargeable lithium-ion batteries, understanding the atomic-scale mechanism of Li-induced structural evolution occurring at the host electrode materials provides essential knowledge for design of new high performance electrodes. Here, we report a new crystalline-crystalline phase transition mechanism in single-crystal Zn-Sb intermetallic nanowires upon lithiation. Using in situ transmission electron microscopy, we observed that stacks of atomic planes in an intermediate hexagonal (h-)LiZnSb phase are "shuffled" to accommodate the geometrical confinement stress arising from lamellar nanodomains intercalated by lithium ions. Such atomic rearrangement arises from the anisotropic lithium diffusion and is accompanied by appearance of partial dislocations. This transient structure mediates further phase transition from h-LiZnSb to cubic (c-)Li2ZnSb, which is associated with a nearly "zero-strain" coherent interface viewed along the [001]h/[111]c directions. This study provides new mechanistic insights into complex electrochemically driven crystalline-crystalline phase transitions in lithium-ion battery electrodes and represents a noble example of atomic-level structural and interfacial rearrangements.

KEYWORDS:

Zn4Sb3 nanowires; atomic scale; in situ STEM; lithium-ion batteries; phase transition

PMID:
25158147
DOI:
10.1021/nl502347z

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