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Combined experimental and computational study of Ce-doped La3Zr2Li7O12 garnet solid-state electrolyte
journal contribution
posted on 2020-02-03, 10:58 authored by Bo Dong, Stephen R Yeandel, Pooja GoddardPooja Goddard, Peter R SlaterLi-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 MaterialsVolume
32Issue
1Pages
215 - 223Publisher
American Chemical Society (ACS)Version
- AM (Accepted Manuscript)
Rights holder
© American Chemical SocietyPublisher 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
2019-12-05Publication date
2019-12-12Copyright date
2019ISSN
0897-4756eISSN
1520-5002Publisher version
Language
- en
Depositor
Dr Pooja Goddard. Deposit date: 1 February 2020Usage metrics
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