%0 Journal Article
%A Helm, Bianca
%A Minafra, Nicolò
%A Wankmiller, Björn
%A Agne, Matthias T.
%A Li, Cheng
%A Senyshyn, Anatoliy
%A Hansen, Michael Ryan
%A Zeier, Wolfgang G.
%T Correlating Structural Disorder to $Li^+$ Ion Transport in $Li_{4–x}Ge_{1–x}Sb_xS_4$ (0 ≤ x ≤ 0.2)
%J Chemistry of materials
%V 34
%N 12
%@ 0897-4756
%C Washington, DC
%I American Chemical Society
%M FZJ-2022-02367
%P  5558–5570
%D 2022
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%U <Go to ISI:>//WOS:000819657500001
%R 10.1021/acs.chemmater.2c00608
%U https://juser.fz-juelich.de/record/908088