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

Published online by Cambridge University Press:  25 May 2018

Kuber Mishra*
Department of Chemical Engineering, University of South Carolina, Columbia, South Carolina 29208, USA
Xiao-Chen Liu
College of Chemistry and Molecular Science, Wuhan University, Wuhan 430072, China
Mark Geppert
Department of Chemical Engineering, University of South Carolina, Columbia, South Carolina 29208, USA
James J. Wu
Electrochemistry Division, NASA Glenn Research Center, Cleveland, Ohio 44135, USA
Jun-Tao Li
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005, China
Ling Huang
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005, China
Shi-Gang Sun
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005, China
Xiao-Dong Zhou*
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005, China; and Department of Chemical Engineering, Institute for Materials Research and Innovation, University of Louisiana, Lafayette, Louisiana 70503, USA
Fu-Sheng Ke*
College of Chemistry and Molecular Science, Wuhan University, Wuhan 430072, China
a)Address all correspondence to these authors. e-mail:
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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.

Copyright © Materials Research Society 2018 

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These authors contributed equally to this work.



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