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Accelerated Reaction Kinetics in Quasi‐Solid‐State Li–S Batteries via Li 10 GeP 2 S 12: From Mechanistic Insights to Pouch Cell Realisation

Abstract:
Lithium–sulfur (Li–S) batteries are emerging as promising next‐generation chemistry due to their ultra‐high energy density, potential for improved safety and the promise of secure global supply chains. Unlike conventional Li–S systems, so‐called quasi‐solid‐state (QSS) Li–S batteries employ electrolytes that sparingly solvate polysulfide species suppressing the ‘shuttle effect’ and enhancing cycling stability. However, to date the practical deployment of QSS cells has been hindered by comparatively sluggish kinetics and limited stability; furthermore, insights into the mechanism of operation of this cell type remain scarce. Here, we demonstrate improved kinetics, through the incorporation of Li10GeP2S12. We explore this performance enhancement by examining degradation pathways using in situ X‐ray computed tomography imaging and complimentary electrochemical techniques. We also propose a concise methodology to quantify the sulfur intermediate according to cyclic voltammetry profiles, revealing the presence of sparingly soluble Li2S x (x = 4.96) and QSS Li2S y (y = 2.53) during cycling in our system. Tomographic imaging clearly identifies morphological evolution during cycling suggesting microscale changes to the electrode as a key cause of capacity decay. Protocols for electrode fabrication, electrolyte preparation, and cell assembly were established, achieving a sulfur loading > 4 mgS cm−2, a capacity > 1200 mAh gS−1, and stability with 2.8% capacity loss over 100 cycles.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1002/batt.70348

Authors

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Role:
Author
ORCID:
0000-0002-6169-3942
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Institution:
University of Oxford
Role:
Author


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Funder identifier:
10.13039/501100000287
Grant:
Grant CiET1718\59
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Funder identifier:
10.13039/100017146
Grant:
Grant FIRG083
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Funder identifier:
https://ror.org/05ar5fy68
Grant:
Grant 10040939
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Funder identifier:
https://ror.org/0526snb40


Publisher:
Wiley
Journal:
Batteries & Supercaps More from this journal
Volume:
9
Issue:
6
Article number:
e70348
Publication date:
2026-06-01
Acceptance date:
2026-05-19
DOI:
EISSN:
2566-6223
ISSN:
2566-6223


Language:
English
Keywords:
Source identifiers:
4101851
Deposit date:
2026-06-01
ARK identifier:
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