Diffusion coefficient of lithium ions in garnet-type Li6.5La3Zr1.5Ta0.5O12 single crystal probed by 7Li pulsed field gradient-NMR spectroscopy

被引:43
作者
Dorai, Arunkumar [1 ]
Kuwata, Naoaki [1 ]
Takekawa, Reiji [1 ]
Kawamura, Junichi [1 ]
Kataoka, Kunimitsu [2 ]
Akimoto, Junji [2 ]
机构
[1] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Aoba Ku, 2-1-1 Katahira, Sendai, Miyagi 9808577, Japan
[2] Natl Inst Adv Ind Sci & Technol, I-1-1 Higashi, Tsukuba, Ibaraki 3058565, Japan
基金
日本学术振兴会;
关键词
Tantalum-doped garnet-type lithium ion conductor; Single crystal; Solid electrolyte; Li diffusion coefficient; PFG-NMR; All-solid-state lithium battery; DOPED LI7LA3ZR2O12; CONDUCTIVITY; CONDUCTORS; AL; RELAXATION; LISICON; TA; GA;
D O I
10.1016/j.ssi.2018.10.016
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Diffusion coefficient of lithium ions in Li6.5La3Zr1.5Ta0.5O12 (LLZTO) single crystal is measured using 'Li pulse( field gradient nuclear magnetic resonance (PFG-NMR) spectroscopy in the temperature range from 298 K tc 353 K. The Li diffusion coefficient in LLZTO is evaluated to be 1.9 x 10(-13) m(2) s(-1) at 298 K with the activation energy of 0.43 eV. The ionic conductivity of LLZTO single crystal is measured by impedance spectroscopy, whicl gives 7 x 10(-4) S cm(-1) at 298 K with the activation energy of 0.43 eV. The diffusion coefficient obtained by PFG NMR is lesser than the diffusion coefficient calculated from ionic conductivity using Nernst-Einstein relation The small discrepancy gives the Haven ratio of 0.4, which suggests a correlated migration of the lithium ions it the tetrahedral and octahedral sites in LLZTO. To compare the present result with previous reports, the diffusior time (d) dependence is carefully checked in PFG-NMR not only for the single crystal but also the crushes powdered samples, which revealed no significant dependence in the single crystal but small dependence in tht crushed samples which may be due to the restricted diffusion in the powder grains.
引用
收藏
页码:18 / 26
页数:9
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