First principles and experimental studies of empty Si46 as anode materials for Li-ion batteries

Kwai S. Chan, Michael A. Miller, Wuwei Liang, Carol Ellis-Terrell, Candace Chan

Research output: Contribution to journalArticlepeer-review

12 Scopus citations


The objective of this investigation was to utilize the first-principles molecular dynamics computational approach to investigate the lithiation characteristics of empty silicon clathrates (Si46) for applications as potential anode materials in lithium-ion batteries. The energy of formation, volume expansion, and theoretical capacity were computed for empty silicon clathrates as a function of Li. The theoretical results were compared against experimental data of long-term cyclic tests performed on half-cells using electrodes fabricated from Si46 prepared using a Hofmann-type elimination-oxidation reaction. The comparison revealed that the theoretically predicted capacity (of 791.6 mAh/g) agreed with experimental data (809 mAh/g) that occurred after insertion of 48 Li atoms. The calculations showed that overlithiation beyond 66 Li atoms can cause large volume expansion with a volume strain as high as 120%, which may correlate to experimental observations of decreasing capacities from the maximum at 1030 mAh/g to 553 mA h/g during long-term cycling tests. The finding suggests that overlithiation beyond 66 Li atoms may have caused damage to the cage structure and led to lower reversible capacities.

Original languageEnglish (US)
Pages (from-to)3657-3665
Number of pages9
JournalJournal of Materials Research
Issue number23
StatePublished - Dec 14 2016


  • Li-ion battery
  • anode materials
  • silicon clathrates

ASJC Scopus subject areas

  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering


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