High Li ion conductivity in a garnet-type solid electrolyte via unusual site occupation of the doping Ca ions

Shufeng Song, Denis Sheptyakov, Alexander M. Korsunsky, Hai M. Duong, Li Lu

Research output: Contribution to journalArticlepeer-review

51 Citations (Scopus)

Abstract

The search for solid electrolytes with high stability and ionic conductivity is a long sought-after goal in the development of safe and high energy density Li-ion batteries. Garnet-type lithium conductors form a most promising family of materials due to their good chemical stability. However, the low conductivity at room temperature prevents wider application of these materials. It has long been recognized that alkaline earth metals are confined exclusively to dodecahedral 8-coordinated sites within the garnet framework. In contrast to this dominant viewpoint, we show that Ca2+ cations can occupy the octahedral 6-coordinated sites, leading to an enhanced room temperature conductivity of 5.2 × 10-4 S cm-1 and reduced activation energy of 0.27 eV, together with a 0 to 9 V electrochemical stability window. This finding opens up a new opportunity for the design of ceramic electrolytes with higher conductivities, providing added impetus for further exploration of oxide electrolyte chemistry.

Original languageEnglish
Pages (from-to)232-237
Number of pages6
JournalMaterials and Design
Volume93
DOIs
Publication statusPublished - 5 Mar 2016
Externally publishedYes

Keywords

  • Alkaline earth doping
  • Conductivity
  • Garnet
  • Neutron diffraction
  • Solid electrolyte

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