Pressure-Induced Dislocations and Their Influence on Ionic Transport in Li+-Conducting Argyrodites

Vasiliki Faka; Matthias T. Agne; Martin A. Lange; Dominik Daisenberger; Björn Wankmiller; Stefan Schwarzmüller; Hubert Huppertz; Oliver Maus; Bianca Helm; Thorben Böger; Johannes Hartel; Josef Maximilian Gerdes; Jamie J. Molaison; Gregor Kieslich; Michael Ryan Hansen; Wolfgang G. Zeier

doi:10.1021/jacs.3c12323

Pressure-Induced Dislocations and Their Influence on Ionic Transport in Li⁺-Conducting Argyrodites

Vasiliki Faka, Matthias T. Agne, Martin A. Lange, Dominik Daisenberger, Björn Wankmiller, Stefan Schwarzmüller, Hubert Huppertz, Oliver Maus, Bianca Helm, Thorben Böger, Johannes Hartel, Josef Maximilian Gerdes, Jamie J. Molaison, Gregor Kieslich, Michael Ryan Hansen, Wolfgang G. Zeier

SNS Science Support 1

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

The influence of the microstructure on the ionic conductivity and cell performance is a topic of broad scientific interest in solid-state batteries. The current understanding is that interfacial decomposition reactions during cycling induce local strain at the interfaces between solid electrolytes and the anode/cathode, as well as within the electrode composites. Characterizing the effects of internal strain on ion transport is particularly important, given the significant local chemomechanical effects caused by volumetric changes of the active materials during cycling. Here, we show the effects of internal strain on the bulk ionic transport of the argyrodite Li₆PS₅Br. Internal strain is reproducibly induced by applying pressures with values up to 10 GPa. An internal permanent strain is observed in the material, indicating long-range strain fields typical for dislocations. With increasing dislocation densities, an increase in the lithium ionic conductivity can be observed that extends into improved ionic transport in solid-state battery electrode composites. This work shows the potential of strain engineering as an additional approach for tuning ion conductors without changing the composition of the material itself.

Original language	English
Pages (from-to)	1710-1721
Number of pages	12
Journal	Journal of the American Chemical Society
Volume	146
Issue number	2
DOIs	https://doi.org/10.1021/jacs.3c12323
State	Published - Jan 17 2024

Funding

The research was supported by the Deutsche Forschungsgemeinschaft (DFG) under grant number ZE 1010/12-1. We further acknowledge funding from the Deutsche Forschungsgemeinschaft under project number 459785385. S. Schwarzmüller also acknowledges funding from the DFG within the Walter Benjamin Programme (SCHW 2168/1-1). This work used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory, and was carried out at BL-3, SNAP instrument (reference no. IPTS-29226.1). Part of this research was carried out with the support of Diamond Light Source, instrument I15 (reference no. CY31791). The authors would also like to thank the beamline scientist Dr. Christopher A. Tulk for his assistance during the neutron measurements and the senior scientist Dr. Malcolm Guthrie for his assistance with reduction of neutron data.

Funders	Funder number
Office of Science	IPTS-29226.1, CY31791
Deutsche Forschungsgemeinschaft	459785385, SCHW 2168/1-1, ZE 1010/12-1

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10.1021/jacs.3c12323

Cite this

Faka, V., Agne, M. T., Lange, M. A., Daisenberger, D., Wankmiller, B., Schwarzmüller, S., Huppertz, H., Maus, O., Helm, B., Böger, T., Hartel, J., Gerdes, J. M., Molaison, J. J., Kieslich, G., Hansen, M. R., & Zeier, W. G. (2024). Pressure-Induced Dislocations and Their Influence on Ionic Transport in Li⁺-Conducting Argyrodites. Journal of the American Chemical Society, 146(2), 1710-1721. https://doi.org/10.1021/jacs.3c12323

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title = "Pressure-Induced Dislocations and Their Influence on Ionic Transport in Li+-Conducting Argyrodites",

abstract = "The influence of the microstructure on the ionic conductivity and cell performance is a topic of broad scientific interest in solid-state batteries. The current understanding is that interfacial decomposition reactions during cycling induce local strain at the interfaces between solid electrolytes and the anode/cathode, as well as within the electrode composites. Characterizing the effects of internal strain on ion transport is particularly important, given the significant local chemomechanical effects caused by volumetric changes of the active materials during cycling. Here, we show the effects of internal strain on the bulk ionic transport of the argyrodite Li6PS5Br. Internal strain is reproducibly induced by applying pressures with values up to 10 GPa. An internal permanent strain is observed in the material, indicating long-range strain fields typical for dislocations. With increasing dislocation densities, an increase in the lithium ionic conductivity can be observed that extends into improved ionic transport in solid-state battery electrode composites. This work shows the potential of strain engineering as an additional approach for tuning ion conductors without changing the composition of the material itself.",

author = "Vasiliki Faka and Agne, {Matthias T.} and Lange, {Martin A.} and Dominik Daisenberger and Bj{\"o}rn Wankmiller and Stefan Schwarzm{\"u}ller and Hubert Huppertz and Oliver Maus and Bianca Helm and Thorben B{\"o}ger and Johannes Hartel and Gerdes, {Josef Maximilian} and Molaison, {Jamie J.} and Gregor Kieslich and Hansen, {Michael Ryan} and Zeier, {Wolfgang G.}",

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Faka, V, Agne, MT, Lange, MA, Daisenberger, D, Wankmiller, B, Schwarzmüller, S, Huppertz, H, Maus, O, Helm, B, Böger, T, Hartel, J, Gerdes, JM, Molaison, JJ, Kieslich, G, Hansen, MR & Zeier, WG 2024, 'Pressure-Induced Dislocations and Their Influence on Ionic Transport in Li⁺-Conducting Argyrodites', Journal of the American Chemical Society, vol. 146, no. 2, pp. 1710-1721. https://doi.org/10.1021/jacs.3c12323

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AU - Faka, Vasiliki

AU - Agne, Matthias T.

AU - Lange, Martin A.

AU - Daisenberger, Dominik

AU - Wankmiller, Björn

AU - Schwarzmüller, Stefan

AU - Huppertz, Hubert

AU - Maus, Oliver

AU - Helm, Bianca

AU - Böger, Thorben

AU - Hartel, Johannes

AU - Gerdes, Josef Maximilian

AU - Molaison, Jamie J.

AU - Kieslich, Gregor

AU - Hansen, Michael Ryan

AU - Zeier, Wolfgang G.

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