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Correlating Structural Disorder to Li+ Ion Transport in Li4–xGe1–xSbxS4 (0 ≤ x ≤ 0.2)
- Source :
- Chemistry of materials 34(12), 5558–5570 (2022). doi:10.1021/acs.chemmater.2c00608
- Publication Year :
- 2022
- Publisher :
- American Chemical Society (ACS), 2022.
-
Abstract
- Strong compositional influences are known to affect the ionic transport within the thio-LISICON family, however, a deeper understanding of the resulting structure - transport correlations have up until now been lacking. Employing a combination of high-resolution neutron diffraction, impedance spectroscopy and nuclear magnetic resonance spectroscopy, together with bond valence site energy calculations and the maximum entropy method for determining the underlying Li+ scattering density distribution of a crystal structure, this work assesses the impact of the Li+ substructure and charge carrier density on the ionic transport within the Li4-xGe1-xSbxS4 substitution series. By incorporating Sb5+ into Li4GeS4, an anisometric expansion of the unit cell is observed. An additional Li+ position is found as soon as (SbS4)3− polyhedra are present, leading to a better local polyhedral connectivity and a higher disorder in the Li+ substructure. Here, we are able to relate structural disorder to an increase in configurational entropy, together with a two order-of-magnitude increase in ionic conductivity. This result reinforces the typically believed paradigm that structural disorder leads to improvements in ionic transport.
- Subjects :
- General Chemical Engineering
ddc:540
Materials Chemistry
General Chemistry
Subjects
Details
- ISSN :
- 15205002 and 08974756
- Volume :
- 34
- Database :
- OpenAIRE
- Journal :
- Chemistry of Materials
- Accession number :
- edsair.doi.dedup.....fc408c3b4b9ce18c0460da8beba16855