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Understanding the Role of Triple Phase Boundaries on Coating-Free Solid-State Cathodes

Abstract:
Sulfide solid electrolytes have high ionic conductivities necessary to achieve high-rate solid-state cathodes at room temperature and low pressure. Cathode active materials generally require coatings to avoid deleterious oxidative decomposition reactions with the electrolyte. Coatings add cost and complexity to the manufacture. Here we decouple the effect of double and triple phase boundaries on the decomposition in the thick (i.e., ∼110 μm) uncoated solid state cathode. We show that more severe oxidative decomposition of solid electrolytes occurs when the cathode active materials, carbon, and the solid electrolyte coexist, highlighting the importance of the triple phase boundary concerning the decomposition. By regulating the electronic pathways at the triple phase boundary, a thick uncoated electrode at 1 mA cm–2 and 2 MPa stack pressure, delivers an initial areal capacity of ∼4.6 mAh cm–2 at 30 °C and ∼85% capacity retention after 500 cycles.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/acsenergylett.5c02607

Authors

More by this author
Institution:
University of Oxford
Division:
SSD
Department:
International Development
Sub department:
Refugee Studies Centre
Role:
Author
ORCID:
0000-0003-0873-7405
More by this author
Institution:
University of Oxford
Division:
SSD
Department:
International Development
Sub department:
Refugee Studies Centre
Role:
Author
ORCID:
0009-0008-8681-7850
More by this author
Institution:
University of Oxford
Division:
SSD
Department:
International Development
Sub department:
Refugee Studies Centre
Role:
Author
ORCID:
0000-0003-0166-6333
More by this author
Institution:
University of Oxford
Division:
SSD
Department:
International Development
Sub department:
Refugee Studies Centre
Role:
Author
More by this author
Institution:
University of Oxford
Division:
SSD
Department:
International Development
Sub department:
Refugee Studies Centre
Role:
Author
ORCID:
0000-0002-4874-9745


More from this funder
Funder identifier:
https://ror.org/052gg0110
Grant:
EP/M02833X/1
More from this funder
Funder identifier:
https://ror.org/01h0zpd94
Grant:
22309110
More from this funder
Funder identifier:
https://ror.org/0439y7842
Grant:
EP/M009521/1
More from this funder
Funder identifier:
10.13039/100017146
Grant:
FIRG007
More from this funder
Funder identifier:
https://ror.org/013a0r905
Grant:
EP/R0066X/1


Publisher:
American Chemical Society
Journal:
ACS Energy Letters More from this journal
Volume:
11
Issue:
2
Pages:
1623-1630
Publication date:
2026-01-30
Acceptance date:
2026-01-27
DOI:
EISSN:
2380-8195
ISSN:
2380-8195


Language:
English
Keywords:
Source identifiers:
3763300
Deposit date:
2026-02-16
ARK identifier:
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