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Orientation-Dependent Interfacial Mobility Governs the Anisotropic Swelling in Lithiated Silicon Nanowires

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† †Department of Engineering Science and Mechanics and ∥Department of Materials Science and Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, United States
‡ Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
§ Center for Integrated Nanotechnologies, Sandia National Laboratories, Albuquerque, New Mexico 87185, United States
⊥ Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
*E-mail: [email protected]; [email protected]; [email protected]
Cite this: Nano Lett. 2012, 12, 4, 1953–1958
Publication Date (Web):March 22, 2012
https://doi.org/10.1021/nl204437t
Copyright © 2012 American Chemical Society
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    Recent independent experiments demonstrated that the lithiation-induced volume expansion in silicon nanowires, nanopillars, and microslabs is highly anisotropic, with predominant expansion along the ⟨110⟩ direction but negligibly small expansion along the ⟨111⟩ direction. The origin of such anisotropic behavior remains elusive. Here, we develop a chemomechanical model to study the phase evolution and morphological changes in lithiated silicon nanowires. The model couples the diffusive reaction of lithium with the lithiation-induced elasto-plastic deformation. We show that the apparent anisotropic swelling is critically controlled by the orientation-dependent mobility of the core–shell interface, i.e., the lithiation reaction rate at the atomically sharp phase boundary between the crystalline core and the amorphous shell. Our results also underscore the importance of structural relaxation by plastic flow behind the moving phase boundary, which is essential to quantitative prediction of the experimentally observed morphologies of lithiated silicon nanowires. The study sheds light on the lithiation-mediated failure in nanowire-based electrodes, and the modeling framework provides a basis for simulating the morphological evolution, stress generation, and fracture in high-capacity electrodes for the next-generation lithium-ion batteries.

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