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Submicro-sized Si-Ge solid solutions with high capacity and long cyclability for lithium-ion batteries

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Abstract

Mastery of strengthening strategies to achieve high-capacity anodes for lithium-ion batteries can shed light on understanding the nature of diffusion-induced stress and offer an approach to use submicro-sized materials with an ultrahigh capacity for large-scale batteries. Here, we report solute strengthening in a series of silicon (Si)—germanium (Ge) alloys. When the larger solute atom (Ge) is added to the solvent atoms (Si), a compressive stress is generated in the vicinity of Ge atoms. This local stress field interacts with resident dislocations and subsequently impedes their motion to increase the yield stress in the alloys. The addition of Ge into Si substantially improves the capacity retention, particularly in Si0.50Ge0.50, aligning with literature reports that the Si/Ge alloy showed a maximum yield stress in Si0.50Ge0.50. In situ X-ray diffraction studies on the Si0.50Ge0.50 electrode show that the phase change undergoes three subsequent steps during the lithiation process: removal of surface oxide layer, formation of cluster-size Lix(Si,Ge), and formation of crystalline Li15(Si,Ge)4. Furthermore, the lithiation process starts from higher index facets, i.e., (220) and (311), then through the low index facet (111), suggesting the orientation-dependence of the lithiation process in the Si0.50Ge0.50 electrode.

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ACKNOWLEDGMENTS

This work was also partially supported by National Science Foundation under Grant No. CBET1408751. Part of the work was sponsored by National Nature Science Foundation of China (21403157) and Natural Science Foundation of Jiangsu Province of China (ZXG201446 and BK20140410) and the Fundamental Research Funds for the Central Universities (2042017kf0232). FSK acknowledges the New Faculty Startup Fund of Wuhan University, Large-scale Instrument and Equipment Sharing Foundation of Wuhan University.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Chemical Engineering, University of South Carolina, Columbia, South Carolina, 29208, USA

    Kuber Mishra & Mark Geppert

  2. College of Chemistry and Molecular Science, Wuhan University, Wuhan, 430072, China

    Xiao-Chen Liu & Fu-Sheng Ke

  3. Electrochemistry Division, NASA Glenn Research Center, Cleveland, Ohio, 44135, USA

    James J. Wu

  4. State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen, 361005, China

    Jun-Tao Li, Ling Huang, Shi-Gang Sun & Xiao-Dong Zhou

  5. Department of Chemical Engineering, Institute for Materials Research and Innovation, University of Louisiana, Lafayette, Louisiana, 70503, USA

    Xiao-Dong Zhou

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  1. Kuber Mishra
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Correspondence to Kuber Mishra, Xiao-Dong Zhou or Fu-Sheng Ke.

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Supplementary Materials: Submicro-Sized Si-Ge Solid Solutions with High Capacity and Long Cyclability for Lithium Ion Batteries (approximately 3.66 MB)

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Mishra, K., Liu, XC., Geppert, M. et al. Submicro-sized Si-Ge solid solutions with high capacity and long cyclability for lithium-ion batteries. Journal of Materials Research 33, 1553–1564 (2018). https://doi.org/10.1557/jmr.2018.145

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