Identifying Hidden Li–Si–O Phases for Lithium-Ion Batteries via First-Principle Thermodynamic Calculations

Jiale Qu, Chao Ning, Xiang Feng, Bonan Yao, Bo Liu, Ziheng Lu, Tianshuai Wang, Zhi Wei Seh, Siqi Shi, Qianfan Zhang

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

SiO–based materials are promising alloys and conversion-type anode materials for lithium-ion batteries and are recently found to be excellent dendrite-proof layers for lithium-metal batteries. However, only a small fraction of the Li–Si–O compositional space has been reported, significantly impeding the understanding of the phase transition mechanisms and the rational design of these materials both as anodes and as protection layers for lithium-metal anodes. Herein, we identify three new thermodynamically stable phases within the Li–Si–O ternary system (Li2SiO5, Li4SiO6, and Li4SiO8) in addition to the existing records via first-principle calculations. The electronic structure simulation shows that Li2SiO5 and Li4SiO8 phases are metallic in nature, ensuring high electronic conductivity required as electrodes. Moduli calculations demonstrate that the mechanical strength of Li–Si–O phases is much higher than that of lithium metal. The diffusion barriers of interstitial Li range from 0.1 to 0.6 eV and the interstitial Li hopping serves as the dominating diffusion mechanism in the Li–Si–O ternary systems compared with vacancy diffusion. These findings provide a new strategy for future discovery of improved alloying anodes for lithium-ion batteries and offer important insight towards the understanding of the phase transformation mechanism of alloy-type protection layers on lithium-metal anodes.

Original languageEnglish
Pages (from-to)865-871
Number of pages7
JournalEnergy and Environmental Materials
Volume5
Issue number3
DOIs
StatePublished - Jul 2022
Externally publishedYes

Keywords

  • anode material
  • crystal structure prediction
  • first-principle calculations
  • ternary alloy phase

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