Li diffusive behavior of garnet-type oxides studied by muon-spin relaxation and QENS

Hiroshi Nozaki; Masashi Harada; Shingo Ohta; Isao Watanabe; Yasuhiro Miyake; Yutaka Ikedo; Niina H. Jalarvo; Eugene Mamontov; Jun Sugiyama

doi:10.1016/j.ssi.2013.10.014

Li diffusive behavior of garnet-type oxides studied by muon-spin relaxation and QENS

Hiroshi Nozaki, Masashi Harada, Shingo Ohta, Isao Watanabe, Yasuhiro Miyake, Yutaka Ikedo, Niina H. Jalarvo, Eugene Mamontov, Jun Sugiyama

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

33 Scopus citations

Abstract

A diffusive behavior of Li⁺ ion in a garnet-type oxide, Li _{5 + x}La₃Zr_xNb_{2 - x}0₁₂ with x = 0-2, has been investigated by both a positive muon-spin relaxation (μ⁺SR) and quasi-elastic neutron scattering (QENS) technique using powder samples. The μ⁺SR results revealed that Li⁺ ions start to diffuse above ~ 150 K for the whole samples measured. The activation energy of Li diffusion (E_a) estimated from the μ⁺SR data was in good agreement with E_a obtained by the QENS measurements. However, both E_as were about a half of E _a of ionic conductivity of Li⁺ (σ_Li), which was evaluated by AC-impedance measurements on sintered pellets. This indicated the serious effect of grain boundary and/or surface on E_a. Furthermore, since the diffusion coefficient of Li⁺ estimated by μ⁺SR is roughly independent of x, the number of mobile Li ⁺ in the garnet lattice was found to be the predominant parameter to determine σ_Li.

Original language	English
Pages (from-to)	585-588
Number of pages	4
Journal	Solid State Ionics
Volume	262
DOIs	https://doi.org/10.1016/j.ssi.2013.10.014
State	Published - Sep 1 2014
Externally published	Yes

Funding

We thank the staff of ISIS, RIKEN/RAL, and J-PARC for help with the μ + SR experiments and the staff of SNS for help with the neutron scattering experiment. This work was supported by the Ultra Slow Muon Microscope (No. 23108003 ) Grant-in Aid for Scientific Research on Innovative Areas from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan.

Keywords

Lithium battery
Muon-spin relaxation
Quasi-elastic neutron scattering
Solid electrolyte

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10.1016/j.ssi.2013.10.014

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title = "Li diffusive behavior of garnet-type oxides studied by muon-spin relaxation and QENS",

abstract = "A diffusive behavior of Li+ ion in a garnet-type oxide, Li 5 + xLa3ZrxNb2 - x012 with x = 0-2, has been investigated by both a positive muon-spin relaxation (μ+SR) and quasi-elastic neutron scattering (QENS) technique using powder samples. The μ+SR results revealed that Li+ ions start to diffuse above ~ 150 K for the whole samples measured. The activation energy of Li diffusion (Ea) estimated from the μ+SR data was in good agreement with Ea obtained by the QENS measurements. However, both Eas were about a half of E a of ionic conductivity of Li+ (σLi), which was evaluated by AC-impedance measurements on sintered pellets. This indicated the serious effect of grain boundary and/or surface on Ea. Furthermore, since the diffusion coefficient of Li+ estimated by μ+SR is roughly independent of x, the number of mobile Li + in the garnet lattice was found to be the predominant parameter to determine σLi.",

keywords = "Lithium battery, Muon-spin relaxation, Quasi-elastic neutron scattering, Solid electrolyte",

author = "Hiroshi Nozaki and Masashi Harada and Shingo Ohta and Isao Watanabe and Yasuhiro Miyake and Yutaka Ikedo and Jalarvo, {Niina H.} and Eugene Mamontov and Jun Sugiyama",

year = "2014",

month = sep,

day = "1",

doi = "10.1016/j.ssi.2013.10.014",

language = "English",

volume = "262",

pages = "585--588",

journal = "Solid State Ionics",

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T1 - Li diffusive behavior of garnet-type oxides studied by muon-spin relaxation and QENS

AU - Nozaki, Hiroshi

AU - Harada, Masashi

AU - Ohta, Shingo

AU - Watanabe, Isao

AU - Miyake, Yasuhiro

AU - Ikedo, Yutaka

AU - Jalarvo, Niina H.

AU - Mamontov, Eugene

AU - Sugiyama, Jun

PY - 2014/9/1

Y1 - 2014/9/1

N2 - A diffusive behavior of Li+ ion in a garnet-type oxide, Li 5 + xLa3ZrxNb2 - x012 with x = 0-2, has been investigated by both a positive muon-spin relaxation (μ+SR) and quasi-elastic neutron scattering (QENS) technique using powder samples. The μ+SR results revealed that Li+ ions start to diffuse above ~ 150 K for the whole samples measured. The activation energy of Li diffusion (Ea) estimated from the μ+SR data was in good agreement with Ea obtained by the QENS measurements. However, both Eas were about a half of E a of ionic conductivity of Li+ (σLi), which was evaluated by AC-impedance measurements on sintered pellets. This indicated the serious effect of grain boundary and/or surface on Ea. Furthermore, since the diffusion coefficient of Li+ estimated by μ+SR is roughly independent of x, the number of mobile Li + in the garnet lattice was found to be the predominant parameter to determine σLi.

AB - A diffusive behavior of Li+ ion in a garnet-type oxide, Li 5 + xLa3ZrxNb2 - x012 with x = 0-2, has been investigated by both a positive muon-spin relaxation (μ+SR) and quasi-elastic neutron scattering (QENS) technique using powder samples. The μ+SR results revealed that Li+ ions start to diffuse above ~ 150 K for the whole samples measured. The activation energy of Li diffusion (Ea) estimated from the μ+SR data was in good agreement with Ea obtained by the QENS measurements. However, both Eas were about a half of E a of ionic conductivity of Li+ (σLi), which was evaluated by AC-impedance measurements on sintered pellets. This indicated the serious effect of grain boundary and/or surface on Ea. Furthermore, since the diffusion coefficient of Li+ estimated by μ+SR is roughly independent of x, the number of mobile Li + in the garnet lattice was found to be the predominant parameter to determine σLi.

KW - Lithium battery

KW - Muon-spin relaxation

KW - Quasi-elastic neutron scattering

KW - Solid electrolyte

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DO - 10.1016/j.ssi.2013.10.014

M3 - Article

AN - SCOPUS:84903311445

SN - 0167-2738

VL - 262

SP - 585

EP - 588

JO - Solid State Ionics

JF - Solid State Ionics

ER -

Li diffusive behavior of garnet-type oxides studied by muon-spin relaxation and QENS

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Keywords

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