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Local Structural Investigations, Defect Formation, and Ionic Conductivity of the Lithium Ionic Conductor Li_4P_2S_6

Dietrich, Christian and Sadowski, Marcel and Sicolo, Sabrina and Weber, Dominik A. and Sedlmaier, Stefan J. and Weldert, Kai S. and Indris, Sylvio and Albe, Karsten and Janek, Jürgen and Zeier, Wolfgang G. (2016):
Local Structural Investigations, Defect Formation, and Ionic Conductivity of the Lithium Ionic Conductor Li_4P_2S_6.
In: Chemistry of Materials, pp. 8764-8773, 28, (23), ISSN 0897-4756,
[Online-Edition: http://doi.org/10.1021/acs.chemmater.6b04175],
[Article]

Abstract

Glassy, glass–ceramic, and crystalline lithium thiophosphates have attracted interest in their use as solid electrolytes in all-solid-state batteries. Despite similar structural motifs, including PS_4^3–, P_2S_6^4–, and P_2S_7^4– polyhedra, these materials exhibit a wide range of possible compositions, crystal structures, and ionic conductivities. Here, we present a combined approach of Bragg diffraction, pair distribution function analysis, Raman spectroscopy, and ^31P magic angle spinning nuclear magnetic resonance spectroscopy to study the underlying crystal structure of Li_4P_2S_6. In this work, we show that the material crystallizes in a planar structural arrangement as a glass ceramic composite, explaining the observed relatively low ionic conductivity, depending on the fraction of glass content. Calculations based on density functional theory provide an understanding of occurring diffusion pathways and ionic conductivity of this Li^+ ionic conductor.

Item Type: Article
Erschienen: 2016
Creators: Dietrich, Christian and Sadowski, Marcel and Sicolo, Sabrina and Weber, Dominik A. and Sedlmaier, Stefan J. and Weldert, Kai S. and Indris, Sylvio and Albe, Karsten and Janek, Jürgen and Zeier, Wolfgang G.
Title: Local Structural Investigations, Defect Formation, and Ionic Conductivity of the Lithium Ionic Conductor Li_4P_2S_6
Language: English
Abstract:

Glassy, glass–ceramic, and crystalline lithium thiophosphates have attracted interest in their use as solid electrolytes in all-solid-state batteries. Despite similar structural motifs, including PS_4^3–, P_2S_6^4–, and P_2S_7^4– polyhedra, these materials exhibit a wide range of possible compositions, crystal structures, and ionic conductivities. Here, we present a combined approach of Bragg diffraction, pair distribution function analysis, Raman spectroscopy, and ^31P magic angle spinning nuclear magnetic resonance spectroscopy to study the underlying crystal structure of Li_4P_2S_6. In this work, we show that the material crystallizes in a planar structural arrangement as a glass ceramic composite, explaining the observed relatively low ionic conductivity, depending on the fraction of glass content. Calculations based on density functional theory provide an understanding of occurring diffusion pathways and ionic conductivity of this Li^+ ionic conductor.

Journal or Publication Title: Chemistry of Materials
Volume: 28
Number: 23
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Materials Modelling
Zentrale Einrichtungen > University IT-Service and Computing Centre (HRZ) > Hochleistungsrechner
11 Department of Materials and Earth Sciences > Material Science
Zentrale Einrichtungen > University IT-Service and Computing Centre (HRZ)
11 Department of Materials and Earth Sciences
Zentrale Einrichtungen
Date Deposited: 18 May 2017 10:30
Official URL: http://doi.org/10.1021/acs.chemmater.6b04175
Identification Number: doi:10.1021/acs.chemmater.6b04175
Funders: The authors acknowledge fi nancial support by BASF SE within the International Network for Electrochemistry and Batteries. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC02-06CH11357. W.G.Z. furthermore gratefully acknowledges the financial support through start-up funding provided by the Justus-Liebig-University Giessen. M.S., S.S., and K.A. acknowledge support by, by the DFG through Project AL-578/19-1 and the computing time granted by the Lichtenberg High Performance Computer of TU Darmstadt within Projects 164 and 273.
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