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The impact of magnesium content on lithium-magnesium alloy electrode performance with argyrodite solid electrolyte

Abstract:
Solid-state lithium-based batteries offer higher energy density than their Li-ion counterparts. Yet they are limited in terms of negative electrode discharge performance and require high stack pressure during operation. To circumvent these issues, we propose the use of lithium-rich magnesium alloys as suitable negative electrodes in combination with Li<sub>6</sub>PS<sub>5</sub>Cl solid-state electrolyte. We synthesise and characterise lithium-rich magnesium alloys, quantifying the changes in mechanical properties, transport, and surface chemistry that impact electrochemical performance. Increases in hardness, stiffness, adhesion, and resistance to creep are quantified by nanoindentation as a function of magnesium content. A decrease in diffusivity is quantified with <sup>6</sup>Li pulsed field gradient nuclear magnetic resonance, and only a small increase in interfacial impedance due to the presence of magnesium is identified by electrochemical impedance spectroscopy which is correlated with x-ray photoelectron spectroscopy. The addition of magnesium aids contact retention on discharge, but this must be balanced against a decrease in lithium diffusivity. We demonstrate via electrochemical testing of symmetric cells at 2.5 MPa and 30<sup>∘</sup>C that 1% magnesium content in the alloy increases the stripping capacity compared to both pure lithium and higher magnesium content alloys by balancing these effects.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1038/s41467-024-48071-0

Authors


More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
ORCID:
0000-0002-6470-3915
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
ORCID:
0000-0001-7026-5010


More from this funder
Funder identifier:
https://ror.org/0439y7842
Grant:
EP/R010145/1


Publisher:
Springer Nature
Journal:
Nature Communications More from this journal
Volume:
15
Issue:
1
Article number:
4511
Place of publication:
England
Publication date:
2024-05-27
Acceptance date:
2024-04-19
DOI:
EISSN:
2041-1723
Pmid:
38802332


Language:
English
Pubs id:
2002189
Local pid:
pubs:2002189
Deposit date:
2024-06-26

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