The role of Li site occupancy on the Li-ion conductivity of Ta-doped Li6.75La3Zr1.75Ta0.25O12 solid electrolyte materials with high Li concentrations

Xingxing Zhang; Cheng Li; Weili Liu; Tae Sik Oh; Jeffrey W. Fergus

doi:10.1016/j.ssi.2021.115713

The role of Li site occupancy on the Li-ion conductivity of Ta-doped Li_6.75La₃Zr_1.75Ta_0.25O₁₂ solid electrolyte materials with high Li concentrations

Xingxing Zhang, Cheng Li, Weili Liu, Tae Sik Oh, Jeffrey W. Fergus

Research output: Contribution to journal › Article › peer-review

8 Scopus citations

Abstract

Garnet-type Li₇La₃Zr₂O₁₂ has attracted much attention because of its promising properties of high ionic conductivity, good chemical stability against Li metal, and good mechanical strength. To better understand the Li conduction mechanism, the Li site occupancy and Li-ion conductivity are studied with a high Li concentration in the range of 6.70–7.15 mol per formula unit. Aluminum and silicon, which presumably were transferred to the sample from the Al₂O₃ crucible during processing, were included in the cubic garnet structure for the Rietveld refinements. The Li-ion conductivity increases with the occupancy of the octahedral Li site (Occupancy: 0.78–0.87, Li-ion conductivity: 3–5 × 10⁻⁴ S/cm). As the lithium content increases, the portion of lithium occupying the 96 h octahedral site increases and that occupying the 24d tetrahedral site decreases.

Original language	English
Article number	115713
Journal	Solid State Ionics
Volume	369
DOIs	https://doi.org/10.1016/j.ssi.2021.115713
State	Published - Oct 15 2021
Externally published	Yes

Funding

This work was supported primarily by NASA under award number NNX15AP44A. A portion of this work used resources at Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The inductively coupled plasma-optical emission spectrometry (ICP-OES) (Perkin Elmer Model Optima 4300DV) at the University of Alabama is acknowledged for the ICP analysis. This work was supported primarily by NASA under award number NNX15AP44A . A portion of this work used resources at Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory . The inductively coupled plasma-optical emission spectrometry (ICP-OES) (Perkin Elmer Model Optima 4300DV) at the University of Alabama is acknowledged for the ICP analysis.

Funders	Funder number
National Aeronautics and Space Administration	NNX15AP44A
Office of Science
Oak Ridge National Laboratory
University of Alabama

Keywords

Garnet electrolytes
Li-ion conductivity
Site occupancy

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.ssi.2021.115713

Cite this

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title = "The role of Li site occupancy on the Li-ion conductivity of Ta-doped Li6.75La3Zr1.75Ta0.25O12 solid electrolyte materials with high Li concentrations",

abstract = "Garnet-type Li7La3Zr2O12 has attracted much attention because of its promising properties of high ionic conductivity, good chemical stability against Li metal, and good mechanical strength. To better understand the Li conduction mechanism, the Li site occupancy and Li-ion conductivity are studied with a high Li concentration in the range of 6.70–7.15 mol per formula unit. Aluminum and silicon, which presumably were transferred to the sample from the Al2O3 crucible during processing, were included in the cubic garnet structure for the Rietveld refinements. The Li-ion conductivity increases with the occupancy of the octahedral Li site (Occupancy: 0.78–0.87, Li-ion conductivity: 3–5 × 10−4 S/cm). As the lithium content increases, the portion of lithium occupying the 96 h octahedral site increases and that occupying the 24d tetrahedral site decreases.",

keywords = "Garnet electrolytes, Li-ion conductivity, Site occupancy",

author = "Xingxing Zhang and Cheng Li and Weili Liu and Oh, {Tae Sik} and Fergus, {Jeffrey W.}",

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T1 - The role of Li site occupancy on the Li-ion conductivity of Ta-doped Li6.75La3Zr1.75Ta0.25O12 solid electrolyte materials with high Li concentrations

AU - Zhang, Xingxing

AU - Li, Cheng

AU - Liu, Weili

AU - Oh, Tae Sik

AU - Fergus, Jeffrey W.

PY - 2021/10/15

Y1 - 2021/10/15

N2 - Garnet-type Li7La3Zr2O12 has attracted much attention because of its promising properties of high ionic conductivity, good chemical stability against Li metal, and good mechanical strength. To better understand the Li conduction mechanism, the Li site occupancy and Li-ion conductivity are studied with a high Li concentration in the range of 6.70–7.15 mol per formula unit. Aluminum and silicon, which presumably were transferred to the sample from the Al2O3 crucible during processing, were included in the cubic garnet structure for the Rietveld refinements. The Li-ion conductivity increases with the occupancy of the octahedral Li site (Occupancy: 0.78–0.87, Li-ion conductivity: 3–5 × 10−4 S/cm). As the lithium content increases, the portion of lithium occupying the 96 h octahedral site increases and that occupying the 24d tetrahedral site decreases.

AB - Garnet-type Li7La3Zr2O12 has attracted much attention because of its promising properties of high ionic conductivity, good chemical stability against Li metal, and good mechanical strength. To better understand the Li conduction mechanism, the Li site occupancy and Li-ion conductivity are studied with a high Li concentration in the range of 6.70–7.15 mol per formula unit. Aluminum and silicon, which presumably were transferred to the sample from the Al2O3 crucible during processing, were included in the cubic garnet structure for the Rietveld refinements. The Li-ion conductivity increases with the occupancy of the octahedral Li site (Occupancy: 0.78–0.87, Li-ion conductivity: 3–5 × 10−4 S/cm). As the lithium content increases, the portion of lithium occupying the 96 h octahedral site increases and that occupying the 24d tetrahedral site decreases.

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