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PreprintCC BYChemRxiv

Impact of SEI Formation History on Lithium Metal Electrode Stability at Elevated Temperatures

  • Yutaro Goto1
  • Yuki Miyaura1
  • Takeru Hamada1
  • Yuta Shiomi1
  • Keiji Shimoda2
  • Chengchao Zhong1
  • Ken-ichi Okazaki3
  • Minoru Kato1
  • Satoshi Yasuno4
  • Tomoaki Kaneko5
  • Keitaro Sodeyama6
  • Masako Suzuki-Sakamaki7
1 more authors
  • Yuki Orikasa1
7 affiliations
  1. 1Department of Applied Chemistry, Ritsumeikan University, 1-1-1, Nojihigashi, Kusatsu, Shiga, Japan, 525-8577
  2. 2Ritsumeikan Global Innovation Research Organization, Ritsumeikan University, 1-1-1, Nojihigashi, Kusatsu, Shiga, Japan, 525-8577
  3. 3Research Organization of Science and Technology, Ritsumeikan University, 1-1-1, Nojihigashi, Kusatsu, Shiga, Japan, 525-8577
  4. 4Japan Synchrotron Radiation Research Institute (JASRI), 1-1-1 Kouto, Sayo, Hyogo, Japan, 679-5198
  5. 5Research organization for Information Science and Technology (RIST), 1-18-16 Hamamatsucho, Minato-ku, Tokyo, Japan, 105-0013
  6. 6Center for Basic Research on Materials, National Institute for Materials Science (NIMS, 1-1 Namiki, Tsukuba, Ibaraki, Japan, 305-0044
  7. 7Graduate School of Engineering, Tohoku University, 6-6, Aramaki Aza Aoba, Aoba-ku, Sendai, Miyagi, Japan, 980-8579
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Abstract

Solid electrolyte interphase (SEI) is critical for stabilizing lithium metal anodes, yet its evolution under thermal stress and the role of its formation history remain poorly understood. Here, lithium plating and stripping on Cu electrodes were investigated in 1.0 and 5.0 M lithium bis(fluorosulfonyl)imide (LiFSI)/propylene carbonate electrolytes at 25 and 80 °C using electrochemical measurements, Raman spectroscopy, hard X-ray photoelectron spectroscopy (HAXPES), and X-ray absorption spectroscopy (XAS). Raman spectra showed that the bulk solvation structure changed little with temperature, whereas HAXPES and XAS revealed that elevated temperature accelerated LiFSI decomposition, inorganic enrichment, and SEI growth, leading to increased interfacial resistance and unstable cycling. Electronic-structure calculations showed that increasing LiFSI concentration enhanced the FSI− contribution to the lowest unoccupied molecular orbital (LUMO), while elevated temperature lowered FSI−-derived unoccupied states, favoring anion reduction. Pre-cycling at room temperature markedly improved subsequent operation at 80 °C, particularly with the concentrated electrolyte. These results demonstrate that high-temperature stability is governed by the combined effects of electrolyte concentration, temperature, and SEI formation history, providing a mechanistic basis for controlling SEI formation and stabilizing lithium plating and stripping under thermal stress.

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Cite

BibTeXRIS
BibTeX
@misc{goto2026impact,
  title = {{Impact of SEI Formation History on Lithium Metal Electrode Stability at Elevated Temperatures}},
  author = {Yutaro Goto and Yuki Miyaura and Takeru Hamada and Yuta Shiomi and Keiji Shimoda and Chengchao Zhong and Ken-ichi Okazaki and Minoru Kato and Satoshi Yasuno and Tomoaki Kaneko and Keitaro Sodeyama and Masako Suzuki-Sakamaki and Yuki Orikasa},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008553/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008553/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Impact of SEI Formation History on Lithium Metal Electrode Stability at Elevated Temperatures
AU  - Yutaro Goto
AU  - Yuki Miyaura
AU  - Takeru Hamada
AU  - Yuta Shiomi
AU  - Keiji Shimoda
AU  - Chengchao Zhong
AU  - Ken-ichi Okazaki
AU  - Minoru Kato
AU  - Satoshi Yasuno
AU  - Tomoaki Kaneko
AU  - Keitaro Sodeyama
AU  - Masako Suzuki-Sakamaki
AU  - Yuki Orikasa
PY  - 2026
DA  - 2026/09/09
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008553/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008553/v1
AB  - Solid electrolyte interphase (SEI) is critical for stabilizing lithium metal anodes, yet its evolution under thermal stress and the role of its formation history remain poorly understood. Here, lithium plating and stripping on Cu electrodes were investigated in 1.0 and 5.0 M lithium bis(fluorosulfonyl)imide (LiFSI)/propylene carbonate electrolytes at 25 and 80 °C using electrochemical measurements, Raman spectroscopy, hard X-ray photoelectron spectroscopy (HAXPES), and X-ray absorption spectroscopy (XAS). Raman spectra showed that the bulk solvation structure changed little with temperature, whereas HAXPES and XAS revealed that elevated temperature accelerated LiFSI decomposition, inorganic enrichment, and SEI growth, leading to increased interfacial resistance and unstable cycling. Electronic-structure calculations showed that increasing LiFSI concentration enhanced the FSI− contribution to the lowest unoccupied molecular orbital (LUMO), while elevated temperature lowered FSI−-derived unoccupied states, favoring anion reduction. Pre-cycling at room temperature markedly improved subsequent operation at 80 °C, particularly with the concentrated electrolyte. These results demonstrate that high-temperature stability is governed by the combined effects of electrolyte concentration, temperature, and SEI formation history, providing a mechanistic basis for controlling SEI formation and stabilizing lithium plating and stripping under thermal stress.
ER  -