Abstract

Tetragonal garnet-type Li7La3Zr2O12 is an important candidate solid electrolyte for all-solid-state lithium ion batteries because of its high ionic conductivity and large electrochemical potential window. Here we employ atomistic simulation methods to show that the most favourable disorder process in Li7La3Zr2O12 involves loss of Li2O resulting in lithium and oxygen vacancies, which promote vacancy mediated self-diffusion. The activation energy for lithium migration (0.45 eV) is much lower than that for oxygen (1.65 eV). Furthermore, the oxygen migration activation energy reveals that the oxygen diffusion in this material can be facilitated at higher temperatures once oxygen vacancies form.

Details

Title
Self-diffusion in garnet-type Li7La3Zr2O12 solid electrolytes
Author
Navaratnarajah, Kuganathan 1 ; Rushton Michael J D 2 ; Grimes, Robin W 3 ; Kilner, John A 4 ; Gkanas, Evangelos I 5 ; Chroneos Alexander 1 

 Imperial College London, Department of Materials, London, UK (GRID:grid.7445.2) (ISNI:0000 0001 2113 8111); Coventry University, Faculty of Engineering, Environment and Computing, Coventry, UK (GRID:grid.8096.7) (ISNI:0000000106754565) 
 Bangor University, Nuclear Futures, Bangor, UK (GRID:grid.7362.0) (ISNI:0000000118820937) 
 Imperial College London, Department of Materials, London, UK (GRID:grid.7445.2) (ISNI:0000 0001 2113 8111) 
 Imperial College London, Department of Materials, London, UK (GRID:grid.7445.2) (ISNI:0000 0001 2113 8111); International Institute for Carbon-Neutral Energy Research (I2CNER) Kyushu University, Fukuoka, Japan (GRID:grid.177174.3) (ISNI:0000 0001 2242 4849) 
 Coventry University, Faculty of Engineering, Environment and Computing, Coventry, UK (GRID:grid.8096.7) (ISNI:0000000106754565) 
Publication year
2021
Publication date
2021
Publisher
Nature Publishing Group
e-ISSN
20452322
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2476791807
Copyright
© The Author(s) 2021. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.