A study of suppressed formation of low-conductivity phases in doped Li7La3Zr2O12 garnets by in situ neutron diffraction

Chen, Yan; Rangasamy, Ezhiylmurugan; dela Cruz, Clarina R.; Liang, Chengdu; An, Ke

doi:10.1039/C5TA04902D

Title: A study of suppressed formation of low-conductivity phases in doped Li₇La₃Zr₂O₁₂ garnets by in situ neutron diffraction

Journal Article · Mon Sep 28 00:00:00 EDT 2015 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/C5TA04902D· OSTI ID:1286868

Chen, Yan ^[1]; Rangasamy, Ezhiylmurugan ^[2]; dela Cruz, Clarina R. ^[3]; Liang, Chengdu ^[2]; An, Ke ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division

Doped Li₇La₃Zr₂O₁₂ garnets, oxide-based solids with good Li⁺ conductivity and compatibility, show great potential as leading electrolyte material candidates for all-solid-state lithium ion batteries. Still yet, the conductive bulk usually suffers from the presence of secondary phases and the transition towards a low-conductivity tetragonal phase during synthesis. Dopants are designed to stabilize the high-conductive cubic phase and suppress the formation of the low-conductivity phases. In situ neutron diffraction enables a direct observation of the doping effects by monitoring the phase evolutions during garnet synthesis. It reveals the reaction mechanism involving the temporary presence of intermediate phases. The off-stoichiometry due to the liquid Li₂CO₃ evaporation leads to the residual of the low-conductivity intermediate phase in the as-synthesized bulk. Appropriate doping of an active element may alter the component of the intermediate phases and promote the completion of the reaction. While the dopants aid to stabilize most of the cubic phase, a small amount of tetragonal phase tends to form under a diffusion process. Lastly, the in situ observations provide the guideline of process optimization to suppress the formation of unwanted low-conductivity phases.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1286868

Journal Information:: Journal of Materials Chemistry. A, Vol. 3, Issue 45; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 45 works

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