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Combined experimental and computational study of Ce-doped La3Zr2Li7O12 garnet solid-state electrolyte

journal contribution
posted on 03.02.2020 by Bo Dong, Stephen R Yeandel, Pooja Goddard, Peter R Slater
Li-containing garnet materials have been attracting considerable interest as potential solid-state electrolytes for Li ion batteries. In such Ln3M2LixO12 (Ln = lanthanide, alkaline earth; M = Zr, Hf, Sn, Nb, Ta, Sb, Bi, Te), the best Li ion conductivity is observed for Li contents, x, just below the maximum 7.0. The decrease in conductivity for x = 7.0 systems is related to Li ordering (cell changes from cubic to tetragonal) to prevent too short Li-Li interactions. In this work, we report a combined experimental and modeling study of Ce4+ doping in La3Zr2Li7O12. We show for the first time that Ce4+ can be doped onto the Zr4+ site in this material. This doping strategy results in a reduction in the tetragonal distortion as well as a lowering of the temperature of the tetragonal-cubic phase transition, attributed to the increase in cell size reducing Li-Li interaction strain. Coupled with these changes, the conductivity shows a significant (1.5 orders of magnitude) improvement. Furthermore, the Ce doping also reduces the interfacial resistance (388 ω cm2 for Li7La3Z1.75Ce025O12) in contact with Li metal, giving additional potential benefits to this doping strategy. The long-term cycling stability of a Li//garnet//Li symmetric cell over 190 h has been demonstrated.

Funding

(EPSRC) Design and high throughput microwave synthesis of Li-ion battery materials : EP/N001982/1

EPSRC grant EP/ R024006/1: ICSF Wave 1: GENESIS: Garnet Electrolytes for New Energy Storage Integrated Solutions

History

School

  • Science

Department

  • Chemistry

Published in

Chemistry of Materials

Volume

32

Issue

1

Pages

215 - 223

Publisher

American Chemical Society (ACS)

Version

AM (Accepted Manuscript)

Rights holder

© American Chemical Society

Publisher statement

This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.chemmater.9b03526.

Acceptance date

05/12/2019

Publication date

2019-12-12

Copyright date

2019

ISSN

0897-4756

eISSN

1520-5002

Language

en

Depositor

Dr Pooja Goddard. Deposit date: 1 February 2020

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