TU Darmstadt / ULB / TUbiblio

Defect thermodynamics and interfacial instability of crystalline Li_4P_2S_6

Sadowski, Marcel and Sicolo, Sabrina and Albe, Karsten (2018):
Defect thermodynamics and interfacial instability of crystalline Li_4P_2S_6.
In: Solid State Ionics, pp. 53-60, 319, ISSN 01672738,
DOI: 10.1016/j.ssi.2018.01.047,
[Online-Edition: https://doi.org/10.1016/j.ssi.2018.01.047],
[Article]

Item Type: Article
Erschienen: 2018
Creators: Sadowski, Marcel and Sicolo, Sabrina and Albe, Karsten
Title: Defect thermodynamics and interfacial instability of crystalline Li_4P_2S_6
Language: English
Journal or Publication Title: Solid State Ionics
Volume: 319
Uncontrolled Keywords: Lithium thiophosphates, Solid electrolyte, Glass-ceramics, Density functional theory, Defect thermodynamics, Interface
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: 06 Feb 2018 12:09
DOI: 10.1016/j.ssi.2018.01.047
Official URL: https://doi.org/10.1016/j.ssi.2018.01.047
Alternative Abstract:
Alternative abstract Language
The defect chemistry of various lithium and sulfur point defects in the solid electrolyte Li_4P_2S_6 in its planar arrangement in the P  3¯1m space group is studied by means of total energy calculations within density functional theory. We show that the formation of Li Frenkel-pairs is the dominant internal defect reaction which provides the charge carriers for ionic conductivity. External sulfur related defect equilibria can be excluded as compensation mechanisms for lithium defects. Moreover, we find that charged lithium interstitials exhibit negative formation energies, pointing to the instability of the electrolyte against metallic lithium. This tendency is supported by total energy calculations that predict a highly exothermic reaction between Li_4P_2S_6 and metallic lithium to give Li_2S and Li_3P. The extent of this interfacial instability is such that we observed substantial reactivity even within static calculations on representative interface models. Depending on the surface orientation, a more or less ordered interphase is formed. The formed interphase shows similarities to Li_2S, which has been suggested to act as a passivating layer that inhibits further reaction between the thiophosphate and metallic lithium.UNSPECIFIED
Export:
Suche nach Titel in: TUfind oder in Google

Optionen (nur für Redakteure)

View Item View Item