Journal
CHEMISTRY OF MATERIALS
Volume 34, Issue 12, Pages 5558-5570Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c00608
Keywords
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Funding
- Federal Ministry of Education and Research (BMBF) [03XP0430F]
- Ministry for Culture and Science of North Rhine Westphalia, Germany
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This study assesses the impact of Li+ substructure and charge carrier density on ionic transport in the Li4-xGe1-xSbxS4 substitution series using various techniques. The results show that structural disorder leads to an increase in configurational entropy and a two-order-of-magnitude increase in ionic conductivity.
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 has up until now been lacking. Employing a combination of highresolution 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 2 order-ofmagnitude increase in ionic conductivity. This result reinforces the typically believed paradigm that structural disorder leads to improvements in ionic transport.
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