Evaluation of the effect of site substitution of Pr doping in the Lithium garnet system Li5La3Nb2O12

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Abstract

Li ion conducting garnets have been attracting considerable interest for use as the electrolyte in all solidstate batteries, due to their high ionic conductivity and wide electrochemical stability window. Consequently, there have been a number of doping studies aimed at optimising the conductivity, focusing on both doping in Li7La3Zr2O12 and Li5La3(Nb/Ta)2O12 systems. In this paper, we report a detailed study of Pr doping in Li5La3Nb2O12, and show that this is a rare example of an ambi-site dopant, being able to be doped onto either the La or Nb site. Interestingly the resultant Pr oxidation state is determined by the site substitution, with oxidation states of 3+ for the La site, and 4+ for the Nb site. While the conductivity is essentially unchanged for the La site substitution, Pr4+ substitution on the Nb site leads to a large increase in the conductivity associated with the increase in Li content (Li5+xLa3Nb2−xPrxO12) up to 0.56 mS cm−1 (at 50 °C) for x = 0.8. Overall, this work highlights the flexibility of these garnet materials to doping, and suggests that further consideration of site substitution be considered for other dopants.
Original languageEnglish
Pages (from-to)10349-10359
Number of pages11
JournalDalton Transactions
Volume49
Issue number30
Early online date29 May 2020
DOIs
Publication statusPublished - 14 Aug 2020

Bibliographical note

Funding Information:
We would like to thank the University of Birmingham for the studentship funding of Mark Stockham and the EPSRC for funding the GENESIS project (under EP/R024006/1). We thank the Diamond Light Source for the award of beam time as part of the Energy Materials Block Allocation Group SP14239. We would also like to thank Prof. Emma Kendrick for the continued use of the dry room facilities. Raw experimental data can be found at: https://doi.org/10.25500/edata.bham.00000490.

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