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Title: Origin of high Li⁺ conduction in doped Li₇La₃Zr₂O₁₂ garnets

Substitution of a native ion in the crystals with a foreign ion that differs in valence (aliovalent doping) has been widely attempted to upgrade solid-state ionic conductors for various charge carriers including O²⁻, H⁺, Li⁺, Na⁺, etc. The doping helps promote the high-conductive framework and dredge the tunnel for fast ion transport. The garnet-type Li₇La₃Zr₂O₁₂ (LLZO) is a fast Li⁺ solid conductor, which received much attention as an electrolyte candidate for all-solid-state lithium ion batteries, showing great potential to offer high energy density and minimize battery safety concerns to meet extensive applications in large energy storage systems such as those for electric vehicles and aerospace. In the Li-stuffed garnet framework of LLZO, the 3D pathway formed by the incompletely occupied tetrahedral sites bridged by a single octahedron enables the superior Li⁺ conductivity. For optimal performance, many aliovalent-doping efforts have been made throughout metal elements (Al³⁺, Ta⁵⁺) and metalloid elements (Ga³⁺, Te⁶⁺) in the periodic table with various valences to stabilize the high-conductive phase and increase the Li vacancy concentration.
 [1] ;  [1] ;  [1] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 16; Journal ID: ISSN 0897-4756
American Chemical Society (ACS)
Research Org:
Oak Ridge National Laboratory (ORNL). Center for Nanophase Materials Sciences (CNMS); Spallation Neutron Source
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States