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Protecting Lithium Metal Electrode With Titanium Based Interphase : Synthesis and Battery Performance

Pakseresht, Sara ; Miikkulainen, Ville ; Ghosalya, Manoj ; Kokkonen, Esko LU orcid ; Sainio, Jani ; Kong, Xiangze ; Urpelainen, Samuli and Kallio, Tanja (2026) In Small Structures 7(3).
Abstract

Atomic layer deposition (ALD) of interphases is a promising strategy for stabilizing lithium metal negative electrode and mitigating dendrite formation in rechargeable batteries. In this work, we investigate the growth mechanism and electrochemical impact of titanium-based ALD coatings on highly reactive lithium surfaces. Operando ambient-pressure X-ray photoelectron spectroscopy (APXPS) was employed to probe the initial stages of a Ti interphase growth under realistic ALD conditions using TiCl4 and H2O precursors. The first H2O pulse rapidly converts the Li surface into LiOH, while subsequent TiCl4 exposure reacts directly with lithium surface to form a stable LiCl interlayer. TiOx... (More)

Atomic layer deposition (ALD) of interphases is a promising strategy for stabilizing lithium metal negative electrode and mitigating dendrite formation in rechargeable batteries. In this work, we investigate the growth mechanism and electrochemical impact of titanium-based ALD coatings on highly reactive lithium surfaces. Operando ambient-pressure X-ray photoelectron spectroscopy (APXPS) was employed to probe the initial stages of a Ti interphase growth under realistic ALD conditions using TiCl4 and H2O precursors. The first H2O pulse rapidly converts the Li surface into LiOH, while subsequent TiCl4 exposure reacts directly with lithium surface to form a stable LiCl interlayer. TiOx nucleates on this LiCl-modified surface, resulting in a composite TiOx/LiCl interphase. This synergistic interphase improves electrolyte wettability, promotes uniform Li+ flux, and suppresses dendritic growth. Electrochemical evaluation shows that TiOx-LiCl-coated Li anodes deliver substantially enhanced interfacial stability and cycling performance. Symmetric cells exhibit stable operation for over 600 h, while full Li‖LiNi0.8Mn0.1Co0.1O2 cells with a 10 ALD cycle TiOx/LiCl coating achieve 100% Coulombic efficiency after 300 charge–discharge cycles at 200 mA g−1, compared with ∼63% for bare lithium. These findings provide mechanistic insight and practical validation of ALD Ti-based coatings as an effective protection strategy for durable lithium metal batteries.

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author
; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
ambient-pressure X-ray photoelectron spectroscopy, atomic layer deposition, dendrite growth, high voltage cathodes, interfacial stability, lithium-metal battery
in
Small Structures
volume
7
issue
3
article number
e202500858
publisher
Wiley
external identifiers
  • scopus:105031372047
ISSN
2688-4062
DOI
10.1002/sstr.202500858
language
English
LU publication?
yes
id
21311d14-f1ae-4785-a7c1-544694e1a086
date added to LUP
2026-03-26 11:16:31
date last changed
2026-03-26 11:16:57
@article{21311d14-f1ae-4785-a7c1-544694e1a086,
  abstract     = {{<p>Atomic layer deposition (ALD) of interphases is a promising strategy for stabilizing lithium metal negative electrode and mitigating dendrite formation in rechargeable batteries. In this work, we investigate the growth mechanism and electrochemical impact of titanium-based ALD coatings on highly reactive lithium surfaces. Operando ambient-pressure X-ray photoelectron spectroscopy (APXPS) was employed to probe the initial stages of a Ti interphase growth under realistic ALD conditions using TiCl<sub>4</sub> and H<sub>2</sub>O precursors. The first H<sub>2</sub>O pulse rapidly converts the Li surface into LiOH, while subsequent TiCl<sub>4</sub> exposure reacts directly with lithium surface to form a stable LiCl interlayer. TiO<sub>x</sub> nucleates on this LiCl-modified surface, resulting in a composite TiO<sub>x</sub>/LiCl interphase. This synergistic interphase improves electrolyte wettability, promotes uniform Li<sup>+</sup> flux, and suppresses dendritic growth. Electrochemical evaluation shows that TiO<sub>x</sub>-LiCl-coated Li anodes deliver substantially enhanced interfacial stability and cycling performance. Symmetric cells exhibit stable operation for over 600 h, while full Li‖LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> cells with a 10 ALD cycle TiO<sub>x</sub>/LiCl coating achieve 100% Coulombic efficiency after 300 charge–discharge cycles at 200 mA g<sup>−1</sup>, compared with ∼63% for bare lithium. These findings provide mechanistic insight and practical validation of ALD Ti-based coatings as an effective protection strategy for durable lithium metal batteries.</p>}},
  author       = {{Pakseresht, Sara and Miikkulainen, Ville and Ghosalya, Manoj and Kokkonen, Esko and Sainio, Jani and Kong, Xiangze and Urpelainen, Samuli and Kallio, Tanja}},
  issn         = {{2688-4062}},
  keywords     = {{ambient-pressure X-ray photoelectron spectroscopy; atomic layer deposition; dendrite growth; high voltage cathodes; interfacial stability; lithium-metal battery}},
  language     = {{eng}},
  number       = {{3}},
  publisher    = {{Wiley}},
  series       = {{Small Structures}},
  title        = {{Protecting Lithium Metal Electrode With Titanium Based Interphase : Synthesis and Battery Performance}},
  url          = {{http://dx.doi.org/10.1002/sstr.202500858}},
  doi          = {{10.1002/sstr.202500858}},
  volume       = {{7}},
  year         = {{2026}},
}