Process-dependent phase evolution in thermally sprayed Li4Ti5O12 thin-film anodes revealed by synchrotron and surface analysis

Arman Hasani; Antti Salminen; Shrikant Joshi; Malgorzata Grazyna Makowska; Behnam Chameh; Vesa Pekka Lehto; Vinay Gidla; Sneha Goel; Ilari Angervo; Ashish Ganvir

doi:10.1016/j.matdes.2026.116414

Process-dependent phase evolution in thermally sprayed Li₄Ti₅O₁₂ thin-film anodes revealed by synchrotron and surface analysis

Arman Hasani^*
, Antti Salminen
, Shrikant Joshi
, Malgorzata Grazyna Makowska
, Behnam Chameh
, Vesa Pekka Lehto
, Vinay Gidla
, Sneha Goel
, Ilari Angervo
, Ashish Ganvir

^*Corresponding author for this work

BA4509 Advanced materials for nuclear energy

University of Turku
University West
Paul Scherrer Institute (PSI)
University of Eastern Finland

Research output: Contribution to journal › Article › Scientific › peer-review

Abstract

Understanding process-induced phase evolution in thermally sprayed Li₄Ti₅O₁₂ (LTO) thin-films is critical for developing scalable battery electrodes with stable electrochemical performance. This study comparatively investigates Atmospheric Plasma Spraying (APS), Suspension Plasma Spraying (SPS), and High-Velocity Oxy-Fuel (HVOF) processing of LTO thin-film anodes using SEM/EDS, laboratory XRD, synchrotron µXRD/µXRF mapping, XPS, and electrochemical characterization. Synchrotron µXRD revealed distinct process-dependent phase evolution governed by thermal exposure and quenching behavior. HVOF retained the highest spinel LTO fraction (66.8 %), APS retained 65.1 %, while SPS showed the strongest decomposition with only 53.5 % LTO together with increased Li₂TiO₃ (43.5 %) and TiO₂ formation (3.0 %). XPS analysis identified Li₂CO₃ surface formation in APS and HVOF coatings, whereas SPS exhibited strong surface lithium depletion. Electrochemical measurements showed that APS-LTO exhibited the most favorable electrochemical response, with a working voltage of ∼1.56 V vs. Li/Li⁺ and lower polarization resistance (∼18.7 kΩ) compared with SPS and HVOF coatings. The results establish process–structure–property relationships linking thermal spray conditions with lithium retention, phase stability, and electrochemical behavior in thermally sprayed LTO thin-films.

Original language	English
Article number	116414
Journal	Materials and Design
Volume	267
DOIs	https://doi.org/10.1016/j.matdes.2026.116414
Publication status	Published - 2026
MoE publication type	A1 Journal article-refereed

Funding

This research was supported by the GREEN-BAT project (2022–2025) under the M-ERA.Net framework. The authors acknowledge funding from the Research Council of Finland, M-ERA.NET 3 through the European Commission, and the national and regional financiers in Germany and Sweden. Prof. Ashish Ganvir acknowledges the SOLACE (DNR 360540) Academy research fellowship, funded by the Research Council of Finland and also extends his gratitude to the City of Turku for supporting his tenure-track grant. The work in Sweden, carried out at University West, received additional support from the NovelCABs proof-of-concept project, funded by the Swedish Energy Agency (Energimyndigheten, Dnr 2021-002227), and from Vinnova, the Swedish Governmental Agency for Innovation Systems, within the M-ERA.NET 3 GREEN-BAT initiative. This project has also received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 958174.

Keywords

Atmospheric plasma spraying
High Velocity Oxy Fuel spraying
LiTiO (LTO)
Process–structure–property correlation
Suspension Plasma Spraying
Synchrotron µXRD and µXRF

Access to Document

10.1016/j.matdes.2026.116414Licence: CC BY

Cite this

@article{67108b0ac52b4a43acc406c4b182b63d,

title = "Process-dependent phase evolution in thermally sprayed Li4Ti5O12 thin-film anodes revealed by synchrotron and surface analysis",

abstract = "Understanding process-induced phase evolution in thermally sprayed Li4Ti5O12 (LTO) thin-films is critical for developing scalable battery electrodes with stable electrochemical performance. This study comparatively investigates Atmospheric Plasma Spraying (APS), Suspension Plasma Spraying (SPS), and High-Velocity Oxy-Fuel (HVOF) processing of LTO thin-film anodes using SEM/EDS, laboratory XRD, synchrotron µXRD/µXRF mapping, XPS, and electrochemical characterization. Synchrotron µXRD revealed distinct process-dependent phase evolution governed by thermal exposure and quenching behavior. HVOF retained the highest spinel LTO fraction (66.8 \%), APS retained 65.1 \%, while SPS showed the strongest decomposition with only 53.5 \% LTO together with increased Li2TiO3 (43.5 \%) and TiO2 formation (3.0 \%). XPS analysis identified Li2CO3 surface formation in APS and HVOF coatings, whereas SPS exhibited strong surface lithium depletion. Electrochemical measurements showed that APS-LTO exhibited the most favorable electrochemical response, with a working voltage of ∼1.56 V vs. Li/Li+ and lower polarization resistance (∼18.7 kΩ) compared with SPS and HVOF coatings. The results establish process–structure–property relationships linking thermal spray conditions with lithium retention, phase stability, and electrochemical behavior in thermally sprayed LTO thin-films.",

keywords = "Atmospheric plasma spraying, High Velocity Oxy Fuel spraying, LiTiO (LTO), Process–structure–property correlation, Suspension Plasma Spraying, Synchrotron µXRD and µXRF",

author = "Arman Hasani and Antti Salminen and Shrikant Joshi and Makowska, \{Malgorzata Grazyna\} and Behnam Chameh and Lehto, \{Vesa Pekka\} and Vinay Gidla and Sneha Goel and Ilari Angervo and Ashish Ganvir",

year = "2026",

doi = "10.1016/j.matdes.2026.116414",

language = "English",

volume = "267",

journal = "Materials and Design",

issn = "0264-1275",

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T1 - Process-dependent phase evolution in thermally sprayed Li4Ti5O12 thin-film anodes revealed by synchrotron and surface analysis

AU - Hasani, Arman

AU - Salminen, Antti

AU - Joshi, Shrikant

AU - Makowska, Malgorzata Grazyna

AU - Chameh, Behnam

AU - Lehto, Vesa Pekka

AU - Gidla, Vinay

AU - Goel, Sneha

AU - Angervo, Ilari

AU - Ganvir, Ashish

PY - 2026

Y1 - 2026

N2 - Understanding process-induced phase evolution in thermally sprayed Li4Ti5O12 (LTO) thin-films is critical for developing scalable battery electrodes with stable electrochemical performance. This study comparatively investigates Atmospheric Plasma Spraying (APS), Suspension Plasma Spraying (SPS), and High-Velocity Oxy-Fuel (HVOF) processing of LTO thin-film anodes using SEM/EDS, laboratory XRD, synchrotron µXRD/µXRF mapping, XPS, and electrochemical characterization. Synchrotron µXRD revealed distinct process-dependent phase evolution governed by thermal exposure and quenching behavior. HVOF retained the highest spinel LTO fraction (66.8 %), APS retained 65.1 %, while SPS showed the strongest decomposition with only 53.5 % LTO together with increased Li2TiO3 (43.5 %) and TiO2 formation (3.0 %). XPS analysis identified Li2CO3 surface formation in APS and HVOF coatings, whereas SPS exhibited strong surface lithium depletion. Electrochemical measurements showed that APS-LTO exhibited the most favorable electrochemical response, with a working voltage of ∼1.56 V vs. Li/Li+ and lower polarization resistance (∼18.7 kΩ) compared with SPS and HVOF coatings. The results establish process–structure–property relationships linking thermal spray conditions with lithium retention, phase stability, and electrochemical behavior in thermally sprayed LTO thin-films.

AB - Understanding process-induced phase evolution in thermally sprayed Li4Ti5O12 (LTO) thin-films is critical for developing scalable battery electrodes with stable electrochemical performance. This study comparatively investigates Atmospheric Plasma Spraying (APS), Suspension Plasma Spraying (SPS), and High-Velocity Oxy-Fuel (HVOF) processing of LTO thin-film anodes using SEM/EDS, laboratory XRD, synchrotron µXRD/µXRF mapping, XPS, and electrochemical characterization. Synchrotron µXRD revealed distinct process-dependent phase evolution governed by thermal exposure and quenching behavior. HVOF retained the highest spinel LTO fraction (66.8 %), APS retained 65.1 %, while SPS showed the strongest decomposition with only 53.5 % LTO together with increased Li2TiO3 (43.5 %) and TiO2 formation (3.0 %). XPS analysis identified Li2CO3 surface formation in APS and HVOF coatings, whereas SPS exhibited strong surface lithium depletion. Electrochemical measurements showed that APS-LTO exhibited the most favorable electrochemical response, with a working voltage of ∼1.56 V vs. Li/Li+ and lower polarization resistance (∼18.7 kΩ) compared with SPS and HVOF coatings. The results establish process–structure–property relationships linking thermal spray conditions with lithium retention, phase stability, and electrochemical behavior in thermally sprayed LTO thin-films.

KW - Atmospheric plasma spraying

KW - High Velocity Oxy Fuel spraying

KW - LiTiO (LTO)

KW - Process–structure–property correlation

KW - Suspension Plasma Spraying

KW - Synchrotron µXRD and µXRF

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