Type I Clathrates as Novel Silicon Anodes: An Electrochemical and Structural Investigation

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

Research output: Contribution to journalArticlepeer-review

27 Scopus citations

Abstract

Silicon clathrates contain cage-like structures that can encapsulate various guest atoms or molecules. An electrochemical evaluation of type I silicon clathrates based on Ba8AlySi46−y as the anode material for lithium-ion batteries is presented here. Postcycling characterization with nuclear magnetic resonance and X-ray diffraction shows no discernible structural or volume changes even after electrochemical insertion of 44 Li (≈1 Li/Si) into the clathrate structure. The observed properties are in stark contrast with lithiation of other silicon anodes, which become amorphous and suffer from large volume changes. The electrochemical reactions are proposed to occur as single phase reactions at approximately 0.2 and 0.4 V versus Li/Li+ during lithiation and delithiation, respectively, distinct from 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 Ba8Al8.54Si37.46, corresponding to ≈1.18 Li/Si. These results show that silicon clathrates could be promising durable anodes for lithium-ion batteries.

Original languageEnglish (US)
Article number1500057
JournalAdvanced Science
Volume2
Issue number6
DOIs
StatePublished - Jun 2015

Keywords

  • Li-ion battery
  • anode
  • silicon
  • ternary type I clathrate

ASJC Scopus subject areas

  • Medicine (miscellaneous)
  • General Chemical Engineering
  • General Materials Science
  • Biochemistry, Genetics and Molecular Biology (miscellaneous)
  • General Engineering
  • General Physics and Astronomy

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