Reaction Front Evolution during Electrochemical Lithiation of Crystalline Silicon Nanopillars

Seok Woo Lee, Lucas A. Berla, Matthew T. McDowell, William D. Nix, Yi Cui

Research output: Contribution to journalArticlepeer-review

18 Scopus citations


The high theoretical specific capacity of Si as an anode material is attractive in lithium-ion batteries, although the issues caused by large volume changes during cycling have been a major challenge. Efforts have been devoted to understanding how diffusion-induced stresses cause fracture, but recent observations of anisotropic volume expansion in single-crystalline Si nanostructures require new theoretical considerations of expansion behavior during lithiation. Further experimental investigation is also necessary to better understand the anisotropy of the lithiation process. Here, we present a method to reveal the crystalline core of partially lithiated Si nanopillars with three different crystallographic orientations by using methanol to dissolve the Li atoms from the amorphous Li-Si alloy. The exposed crystalline cores have flat {110} surfaces at the pillar sidewalls; these surfaces represent the position of the reaction front between the crystalline core and the amorphous Li-Si alloy. It was also found that an amorphous Si structure remained on the flat surfaces of the crystalline core after dissolution of the Li, which was presumed to be caused by the accumulation of Si atoms left over from the removal of Li from the Li-Si alloy. © 2012 Wiley-VCH Verlag GmbH &Co. KGaA, Weinheim.
Original languageEnglish (US)
Pages (from-to)1118-1123
Number of pages6
JournalIsrael Journal of Chemistry
Issue number11-12
StatePublished - Dec 11 2012
Externally publishedYes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): KUK-F1-038-02
Acknowledgements: A portion of this work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Contract No. DE-AC02-76SF00515 through the SLAC National Accelerator Laboratory LDRD Project and Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, Subcontract No. 6951379 under the Batteries for Advanced Transportation Technologies (BATT) Program. S. W. L. acknowledges support from KAUST (No. KUK-F1-038-02). M. T. M. acknowledges support from the Chevron Stanford Graduate Fellowship, the National Defense Science and Engineering Graduate Fellowship, and the National Science Foundation Graduate Fellowship. L. A. B. acknowledges support from the National Science Foundation Graduate Research Fellowship and together with W.D.N. gratefully acknowledges support from the Office of Science, Office of Basic Energy Sciences, of the U. S. Department of Energy under Contract No. DE-FG02-04ER46163.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.


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