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Rapid scalable plasma processing of thin-film Li–La–Zr–O solid-state electrolytes

Crane, Gabriel Badillo ; Colburn, Thomas W. ; Holmes, Sarah E. ; Just, Justus LU orcid ; Cui, Yi and Dauskardt, Reinhold H. (2025) In Matter 8(11).
Abstract

Solid-state electrolytes, such as lithium lanthanum zirconium oxide (LLZO), show promise as technologies for next-generation high-energy-density batteries, but commercial development has been hindered by a lack of scalable processing methods. Current fabrication methods are costly or require long annealing steps to create dense films. We report an atmospheric pressure blown-arc nitrogen plasma jet process to rapidly form sub-micrometer-thick, dense amorphous LLZO (a-LLZO) films from sol-gel precursors. Films are processed in less than 2 min, an order of magnitude faster than what has previously been reported. We demonstrate 500-nm-thick a-LLZO films processed at 350°C with an ionic conductivity of 2 × 10−6 S/cm at 30°C and 2... (More)

Solid-state electrolytes, such as lithium lanthanum zirconium oxide (LLZO), show promise as technologies for next-generation high-energy-density batteries, but commercial development has been hindered by a lack of scalable processing methods. Current fabrication methods are costly or require long annealing steps to create dense films. We report an atmospheric pressure blown-arc nitrogen plasma jet process to rapidly form sub-micrometer-thick, dense amorphous LLZO (a-LLZO) films from sol-gel precursors. Films are processed in less than 2 min, an order of magnitude faster than what has previously been reported. We demonstrate 500-nm-thick a-LLZO films processed at 350°C with an ionic conductivity of 2 × 10−6 S/cm at 30°C and 2 × 10−3 S/cm at 100°C and a conductance of 19 S at 100°C, the highest conductance of any LLZO phase to date. The films exhibit outstanding smooth surface morphology with low defectivity, advancing atmospheric plasma processing as a scalable processing method for solid-state electrolytes.

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
a-LLZO, amorphous electrolytes, EXAFS, LLZO, plasma curing, scalable manufacturing, separator films, solid-state batteries, thin film, XANES
in
Matter
volume
8
issue
11
article number
102468
publisher
Cell Press
external identifiers
  • scopus:105017613038
ISSN
2590-2393
DOI
10.1016/j.matt.2025.102468
language
English
LU publication?
yes
id
b76df33a-f2c9-42d5-8db7-7210c3595b82
date added to LUP
2025-12-08 11:41:54
date last changed
2025-12-08 11:42:47
@article{b76df33a-f2c9-42d5-8db7-7210c3595b82,
  abstract     = {{<p>Solid-state electrolytes, such as lithium lanthanum zirconium oxide (LLZO), show promise as technologies for next-generation high-energy-density batteries, but commercial development has been hindered by a lack of scalable processing methods. Current fabrication methods are costly or require long annealing steps to create dense films. We report an atmospheric pressure blown-arc nitrogen plasma jet process to rapidly form sub-micrometer-thick, dense amorphous LLZO (a-LLZO) films from sol-gel precursors. Films are processed in less than 2 min, an order of magnitude faster than what has previously been reported. We demonstrate 500-nm-thick a-LLZO films processed at 350°C with an ionic conductivity of 2 × 10<sup>−6</sup> S/cm at 30°C and 2 × 10<sup>−3</sup> S/cm at 100°C and a conductance of 19 S at 100°C, the highest conductance of any LLZO phase to date. The films exhibit outstanding smooth surface morphology with low defectivity, advancing atmospheric plasma processing as a scalable processing method for solid-state electrolytes.</p>}},
  author       = {{Crane, Gabriel Badillo and Colburn, Thomas W. and Holmes, Sarah E. and Just, Justus and Cui, Yi and Dauskardt, Reinhold H.}},
  issn         = {{2590-2393}},
  keywords     = {{a-LLZO; amorphous electrolytes; EXAFS; LLZO; plasma curing; scalable manufacturing; separator films; solid-state batteries; thin film; XANES}},
  language     = {{eng}},
  number       = {{11}},
  publisher    = {{Cell Press}},
  series       = {{Matter}},
  title        = {{Rapid scalable plasma processing of thin-film Li–La–Zr–O solid-state electrolytes}},
  url          = {{http://dx.doi.org/10.1016/j.matt.2025.102468}},
  doi          = {{10.1016/j.matt.2025.102468}},
  volume       = {{8}},
  year         = {{2025}},
}