Type I clathrates as novel silicon anodes: An electrochemical and structural investigation

Li, Ying; Raghavan, Rahul; Wagner, Nicholas A.; Davidowski, Stephen K.; Baggetto, Loic; Zhao, Ran; Cheng, Qian; Yarger, Jeffery L.; Veith, Gabriel M.; Ellis-Terrell, Carol; Miller, Michael A.; Chan, Kwai S.; Chan, Candace K.

doi:10.1002/advs.201500057

Title: Type I clathrates as novel silicon anodes: An electrochemical and structural investigation

Journal Article · 05 May 2015 · Advanced Science

DOI: https://doi.org/10.1002/advs.201500057 · OSTI ID:1185934

Li, Ying ^[1]; Raghavan, Rahul ^[1]; Wagner, Nicholas A. ^[1]; Davidowski, Stephen K. ^[1]; Baggetto, Loic ^[2]; Zhao, Ran ^[1]; Cheng, Qian ^[1]; Yarger, Jeffery L. ^[1]; Veith, Gabriel M. ^[2]; Ellis-Terrell, Carol ^[3]; Miller, Michael A. ^[3]; Chan, Kwai S. ^[3]; Chan, Candace K. ^[1]

Arizona State Univ., Tempe, AZ (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Southwest Research Institute, San Antonio, TX (United States)

In this study, silicon clathrates contain cage-like structures that can encapsulate various guest atoms or molecules. Here we present an electrochemical evaluation of type I silicon clathrates based on Ba₈Al_ySi_46-y for the anode material in lithium-ion batteries. Post-cycling characterization with NMR and XRD show no discernible structural or volume changes even after electrochemical insertion of 44 Li into the clathrate structure. The observed properties are in stark contrast with lithiation of other silicon anodes, which become amorphous and suffer from larger volume changes. The lithiation/delithiation processes are proposed to occur in single phase reactions at approximately 0.2 and 0.4 V vs. Li/Li⁺, respectively, distinct from other diamond cubic or amorphous silicon anodes. Reversible capacities as high as 499 mAh g^-1 at a 5 mA g^-1 rate were observed for silicon clathrate with composition Ba₈Al_8.54S_i37.46, corresponding to Li:Si of 1.18:1. The results show that silicon clathrates could be promising durable anodes for lithium-ion batteries.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1185934

Journal Information:: Advanced Science, Vol. 2, Issue 6; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 44 works

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Synthesis, Crystal Structure, and Physical Properties of the Type-I Clathrate Ba _8−δ Ni _x □ _y Si _{46– x – y} Aydemir, U.; Candolfi, C.; Ormeci, A. Inorganic Chemistry, Vol. 51, Issue 8 https://doi.org/10.1021/ic2027626	journal	March 2012
Synthesis, Structure, and High-Temperature Thermoelectric Properties of Boron-Doped Ba ₈ Al ₁₄ Si ₃₁ Clathrate I Phases Condron, Cathie L.; Kauzlarich, Susan M.; Ikeda, Teruyuki Inorganic Chemistry, Vol. 47, Issue 18 https://doi.org/10.1021/ic800772m	journal	September 2008
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High-Pressure Synthesis of a New Silicon Clathrate Superconductor, Ba ₈ Si ₄₆ Yamanaka, Shoji; Enishi, Eiji; Fukuoka, Hiroshi Inorganic Chemistry, Vol. 39, Issue 1 https://doi.org/10.1021/ic990778p	journal	January 2000
Pair Distribution Function Analysis and Solid State NMR Studies of Silicon Electrodes for Lithium Ion Batteries: Understanding the (De)lithiation Mechanisms Key, Baris; Morcrette, Mathieu; Tarascon, Jean-Marie Journal of the American Chemical Society, Vol. 133, Issue 3 https://doi.org/10.1021/ja108085d	journal	January 2011
Arrays of Sealed Silicon Nanotubes As Anodes for Lithium Ion Batteries Song, Taeseup; Xia, Jianliang; Lee, Jin-Hyon Nano Letters, Vol. 10, Issue 5, p. 1710-1716 https://doi.org/10.1021/nl100086e	journal	May 2010
Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation Liu, Xiao Hua; Zheng, He; Zhong, Li Nano Letters, Vol. 11, Issue 8, p. 3312-3318 https://doi.org/10.1021/nl201684d	journal	August 2011
Orientation-Dependent Interfacial Mobility Governs the Anisotropic Swelling in Lithiated Silicon Nanowires Yang, Hui; Huang, Shan; Huang, Xu Nano Letters, Vol. 12, Issue 4 https://doi.org/10.1021/nl204437t	journal	January 2012
Three-Dimensional Metal Scaffold Supported Bicontinuous Silicon Battery Anodes Zhang, Huigang; Braun, Paul V. Nano Letters, Vol. 12, Issue 6 https://doi.org/10.1021/nl204551m	journal	May 2012
Silicon Nanotube Battery Anodes Park, Mi-Hee; Kim, Min Gyu; Joo, Jaebum Nano Letters, Vol. 9, Issue 11, p. 3844-3847 https://doi.org/10.1021/nl902058c	journal	November 2009
Prelithiated Silicon Nanowires as an Anode for Lithium Ion Batteries Liu, Nian; Hu, Liangbing; McDowell, Matthew T. ACS Nano, Vol. 5, Issue 8 https://doi.org/10.1021/nn2017167	journal	July 2011
High-performance lithium-ion anodes using a hierarchical bottom-up approach Magasinski, A.; Dixon, P.; Hertzberg, B. Nature Materials, Vol. 9, Issue 4, p. 353-358 https://doi.org/10.1038/nmat2725	journal	March 2010
Stable cycling of double-walled silicon nanotube battery anodes through solid–electrolyte interphase control Wu, Hui; Chan, Gerentt; Choi, Jang Wook Nature Nanotechnology, Vol. 7, Issue 5 https://doi.org/10.1038/nnano.2012.35	journal	March 2012
Structural characterization of the lithium silicides Li15Si4, Li13Si4, and Li7Si3 using solid state NMR Dupke, Sven; Langer, Thorsten; Pöttgen, Rainer Physical Chemistry Chemical Physics, Vol. 14, Issue 18 https://doi.org/10.1039/c2cp24131e	journal	January 2012

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