Journal of the American Chemical Society, volume 144, issue 22, pages 9597-9609

Ionic Conductivity of Nanocrystalline and Amorphous Li₁₀GeP₂S₁₂: The Detrimental Impact of Local Disorder on Ion Transport

Lukas Schweiger ¹

Katharina Hogrefe ¹

B. Gadermaier ¹

Jennifer L. Rupp ^{2, 3}

Martin Wilkening ¹

Hide authors affiliations Show authors affiliations: 3 affiliations

Institute of Chemistry and Technology of Materials, Christian Doppler Laboratory for Lithium Batteries, Graz University of Technology (NAWI Graz), Graz 8010, Austria |

Electrochemical Materials, Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States |

Electrochemical Materials, Department of Electrical Engineering & Computer Science, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States |

Publication type: Journal Article

Publication date: 2022-05-24

American Chemical Society (ACS)

Journal: Journal of the American Chemical Society

Quartile SCImago

Quartile WOS

Impact factor: 15

ISSN: 00027863, 15205126

DOI: 10.1021/jacs.1c13477

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General Chemistry

Catalysis

Biochemistry

Colloid and Surface Chemistry

Abstract

Solids with extraordinarily high Li+ dynamics are key for high performance all-solid-state batteries. The thiophosphate Li10GeP2S12 (LGPS) belongs to the best Li-ion conductors with an ionic conductivity exceeding 10 mS cm-1 at ambient temperature. Recent molecular dynamics simulations performed by Dawson and Islam predict that the ionic conductivity of LGPS can be further enhanced by a factor of 3 if local disorder is introduced. As yet, no experimental evidence exists supporting this fascinating prediction. Here, we synthesized nanocrystalline LGPS by high-energy ball-milling and probed the Li+ ion transport parameters. Broadband conductivity spectroscopy in combination with electric modulus measurements allowed us to precisely follow the changes in Li+ dynamics. Surprisingly and against the behavior of other electrolytes, bulk ionic conductivity turned out to decrease with increasing milling time, finally leading to a reduction of σ20°C by a factor of 10. 31P, 6Li NMR, and X-ray diffraction showed that ball-milling forms a structurally heterogeneous sample with nm-sized LGPS crystallites and amorphous material. At -135 °C, electrical relaxation in the amorphous regions is by 2 to 3 orders of magnitude slower. Careful separation of the amorphous and (nano)crystalline contributions to overall ion transport revealed that in both regions, Li+ ion dynamics is slowed down compared to untreated LGPS. Hence, introducing defects into the LGPS bulk structure via ball-milling has a negative impact on ionic transport. We postulate that such a kind of structural disorder is detrimental to fast ion transport in materials whose transport properties rely on crystallographically well-defined diffusion pathways.

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Wiley	Wiley, 10, 28.57% Wiley 10 publications, 28.57%
American Chemical Society (ACS)	American Chemical Society (ACS), 7, 20% American Chemical Society (ACS) 7 publications, 20%
Elsevier	Elsevier, 7, 20% Elsevier 7 publications, 20%
Royal Society of Chemistry (RSC)	Royal Society of Chemistry (RSC), 2, 5.71% Royal Society of Chemistry (RSC) 2 publications, 5.71%
Frontiers Media S.A.	Frontiers Media S.A., 2, 5.71% Frontiers Media S.A. 2 publications, 5.71%
IOP Publishing	IOP Publishing, 1, 2.86% IOP Publishing 1 publication, 2.86%
The Electrochemical Society of Japan	The Electrochemical Society of Japan, 1, 2.86% The Electrochemical Society of Japan 1 publication, 2.86%
Cambridge University Press	Cambridge University Press, 1, 2.86% Cambridge University Press 1 publication, 2.86%
American Association for the Advancement of Science (AAAS)	American Association for the Advancement of Science (AAAS), 1, 2.86% American Association for the Advancement of Science (AAAS) 1 publication, 2.86%
Walter de Gruyter	Walter de Gruyter, 1, 2.86% Walter de Gruyter 1 publication, 2.86%
Multidisciplinary Digital Publishing Institute (MDPI)	Multidisciplinary Digital Publishing Institute (MDPI), 1, 2.86% Multidisciplinary Digital Publishing Institute (MDPI) 1 publication, 2.86%
Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii	Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii, 1, 2.86% Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii 1 publication, 2.86%
	2 4 6 8 10

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Schweiger L. et al. Ionic Conductivity of Nanocrystalline and Amorphous Li10GeP2S12: The Detrimental Impact of Local Disorder on Ion Transport // Journal of the American Chemical Society. 2022. Vol. 144. No. 22. pp. 9597-9609.

GOST all authors (up to 50) Copy

Schweiger L., Hogrefe K., Gadermaier B., Rupp J. L., Wilkening M. Ionic Conductivity of Nanocrystalline and Amorphous Li10GeP2S12: The Detrimental Impact of Local Disorder on Ion Transport // Journal of the American Chemical Society. 2022. Vol. 144. No. 22. pp. 9597-9609.

RIS |

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RIS Copy

TY - JOUR

DO - 10.1021/jacs.1c13477

UR - https://doi.org/10.1021/jacs.1c13477

TI - Ionic Conductivity of Nanocrystalline and Amorphous Li10GeP2S12: The Detrimental Impact of Local Disorder on Ion Transport

T2 - Journal of the American Chemical Society

AU - Schweiger, Lukas

AU - Hogrefe, Katharina

AU - Gadermaier, B.

AU - Rupp, Jennifer L.

AU - Wilkening, Martin

PY - 2022

DA - 2022/05/24 00:00:00

PB - American Chemical Society (ACS)

SP - 9597-9609

IS - 22

VL - 144

SN - 0002-7863

SN - 1520-5126

ER -

BibTex |

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BibTex Copy

@article{2022_Schweiger,

author = {Lukas Schweiger and Katharina Hogrefe and B. Gadermaier and Jennifer L. Rupp and Martin Wilkening},

title = {Ionic Conductivity of Nanocrystalline and Amorphous Li10GeP2S12: The Detrimental Impact of Local Disorder on Ion Transport},

journal = {Journal of the American Chemical Society},

year = {2022},

volume = {144},

publisher = {American Chemical Society (ACS)},

month = {may},

url = {https://doi.org/10.1021/jacs.1c13477},

number = {22},

pages = {9597--9609},

doi = {10.1021/jacs.1c13477}

}

MLA

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Schweiger, Lukas, et al. “Ionic Conductivity of Nanocrystalline and Amorphous Li10GeP2S12: The Detrimental Impact of Local Disorder on Ion Transport.” Journal of the American Chemical Society, vol. 144, no. 22, May. 2022, pp. 9597-9609. https://doi.org/10.1021/jacs.1c13477.

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Publisher

American Chemical Society (ACS)

Journal

Journal of the American Chemical Society

Quartile SCImago

Quartile WOS

Impact factor

ISSN

00027863 (Print)
15205126 (Electronic)