Choi, Y-S;
Park, J-H;
Ahn, J-P;
Lee, J-C;
(2017)
Interfacial Reactions in the Li/Si diffusion couples: Origin of Anisotropic Lithiation of Crystalline Si in Li–Si batteries.
Scientific Reports
, 7
(1)
10.1038/s41598-017-14374-0.
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Abstract
As opposed to the common understanding that difusion into a cubic-structured single crystal is independent of its crystalline orientation, the difusion of Li to crystalline Si (c-Si) is anisotropic, which acts as the major cause for the fracture of Si anodes in Li-ion batteries. Here, by conducting comprehensive/multi-scale simulation studies based on molecular dynamics and density functional theory, we elucidate how and why Li difusion in c-Si is anisotropic. We found that Li ions difuse to c-Si by following a particular atomic-scale space corresponding to the lowest value of the valence orbital in c-Si, causing Li ions to take a tortuous difusion pathway. The degree of the tortuosity of the pathway difers depending on the crystallographic orientation of Si, and it acts as the major cause for anisotropic lithiation. We also develop a structural parameter that can quantitatively evaluate the orientation dependency of the lithiation of c-Si.
| Type: | Article |
|---|---|
| Title: | Interfacial Reactions in the Li/Si diffusion couples: Origin of Anisotropic Lithiation of Crystalline Si in Li–Si batteries |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41598-017-14374-0 |
| Publisher version: | http://dx.doi.org/10.1038/s41598-017-14374-0 |
| Language: | English |
| Additional information: | Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
| Keywords: | Batteries, Computational methods, Electronic structure |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10108899 |
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