Journal article
How multi-length scale disorder shapes ion transport in lithium argyrodites
- Abstract:
- The rate performance of all-solid-state batteries can be limited by the low conductivity of the solid electrolyte in the composite cathode. A conductivity of 10 mS cm−1 is required, which exceeds that of many solid electrolytes. This limitation can be attributed to intra- and inter-grain ion transport. Understanding the limitations of ion transport is a multi-length scale problem ranging from single bond hops to particle–particle transport. Here we show that spark plasma sintering of Li6PS5Cl not only enhances ion transport on the macroscopic length scale but also on the microscopic scale. On the macroscopic length scale, greater densification improves particle-to-particle contact. On the nanoscale, short-range order (SRO) of the neighbouring 4a/4a and 4d/4d Wyckoff sites present in the cold-pressed Li6PS5Cl produces unfavourable Li ion pathways through the cell. Spark plasma heating removes the SRO, creating a connected network of microscopic pathways for the Li to migrate. Finally, on the atomistic level, spark plasma heating increases the amount of Cl− residing on the 4d site and S2− on the 4a site. By understanding the limitations of ion mobility across a range of length scales, one can target methods to produce solid-state argyrodite electrolytes with higher ionic conductivities.
- Publication status:
- Published
- Peer review status:
- Peer reviewed
Actions
Access Document
- Files:
-
-
(Preview, Version of record, pdf, 5.8MB, Terms of use)
-
- Publisher copy:
- 10.1039/d5ee01612f
Authors
- Publisher:
- Royal Society of Chemistry
- Journal:
- Energy & Environmental Science More from this journal
- Publication date:
- 2025-08-22
- Acceptance date:
- 2025-08-19
- DOI:
- EISSN:
-
1754-5706
- ISSN:
-
1754-5692
- Language:
-
English
- Pubs id:
-
2287644
- Local pid:
-
pubs:2287644
- Source identifiers:
-
3251036
- Deposit date:
-
2025-09-02
- ARK identifier:
This ORA record was generated from metadata provided by an external service. It has not been edited by the ORA Team.
Terms of use
- Copyright date:
- 2025
- Licence:
- CC Attribution (CC BY) 3.0
If you are the owner of this record, you can report an update to it here: Report update to this record