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Abstract
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 Li7La3Z1.75Ce0.25O12) 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.
Original language | English |
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Pages (from-to) | 215-223 |
Number of pages | 9 |
Journal | Chemistry of Materials |
Volume | 32 |
Issue number | 1 |
Early online date | 12 Dec 2019 |
DOIs | |
Publication status | Published - 14 Jan 2020 |
ASJC Scopus subject areas
- Chemistry(all)
- Chemical Engineering(all)
- Materials Chemistry
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Dive into the research topics of 'Combined experimental and computational study of Ce-doped La3Zr2Li7O12 garnet solid state electrolyte'. Together they form a unique fingerprint.Projects
- 1 Finished
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ICSF Wave 1: GENESIS: Garnet Electrolytes for New Energy Storage Integrated Solutions
Engineering & Physical Science Research Council
1/10/17 → 28/02/21
Project: Research Councils
Datasets
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Combined experimental and computational study of Ce-doped La3Zr2Li7O12 garnet solid state electrolyte
Dong, B. (Creator), Yeandel, S. (Creator), Goddard, P. (Creator) & Slater, P. (Creator), University of Birmingham, 2019
DOI: 10.25500/edata.bham.00000402
Dataset