X射线晶体学
离子
结晶学
锗
材料科学
化学
原子物理学
物理
衍射
硅
光电子学
量子力学
光学
作者
Bianca Helm,Nicolò Minafra,Björn Wankmiller,Matthias T. Agne,Cheng Li,Anatoliy Senyshyn,Michael Ryan Hansen,Wolfgang G. Zeier
标识
DOI:10.1021/acs.chemmater.2c00608
摘要
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 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 2 order-of-magnitude increase in ionic conductivity. This result reinforces the typically believed paradigm that structural disorder leads to improvements in ionic transport.
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