論文 Operando Time-of-Flight Secondary Ion Mass Spectrometry Visualization of Reversible and Irreversible Reactions in Oxide-Based Solid-State Batteries

Sihao Xing ; Gen Hasegawa SAMURAI ORCID ; Prince Sharma ; Daisuke Ito ORCID ; Kazuhiro Kamiguchi ; Kazunori Takada SAMURAI ORCID ; Naoaki Kuwata SAMURAI ORCID

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Sihao Xing, Gen Hasegawa, Prince Sharma, Daisuke Ito, Kazuhiro Kamiguchi, Kazunori Takada, Naoaki Kuwata. Operando Time-of-Flight Secondary Ion Mass Spectrometry Visualization of Reversible and Irreversible Reactions in Oxide-Based Solid-State Batteries. ACS Energy Letters. 2026, 11 (2), 1889-1896. https://doi.org/10.1021/acsenergylett.5c03610

説明:

(abstract)

Operando time-of-flight secondary ion mass spectrometry (TOF-SIMS) was applied to solid-state batteries (SSBs) to visualize dynamic electrode reactions. The SSBs consist of a LiNi0.8Co0.15Al0.05O2 (NCA) composite positive electrode, a Li4Ti5O12 (LTO) composite negative electrode, and a Li2OHCl0.9F0.1/Li0.31La0.56TiO3 composite solid electrolyte, which were fabricated by a pressure-assisted melt infiltration method. Reversible changes in 6Li+, 58Ni+, and 48Ti+ intensities were observed during charge–discharge processes. The intensity change of transition metal secondary ions is attributed to changes in ionization efficiency (matrix effects) and correlates with the state of charge. Reaction inhomogeneity was detected in the NCA composite electrode, indicating that the solid electrolyte infiltration has a positive effect on the electrochemical performance, whereas the LTO electrode exhibited uniform reaction distribution. These findings demonstrate that operando TOF-SIMS can provide critical insights into reaction distribution and irreversible capacity in SSBs, thereby guiding the optimization of electrode architectures.

全固体電池の内部で起こる電極反応を、その場で観察するために、Operando TOF-SIMS（飛行時間型二次イオン質量分析法）を用いました。試作した全固体電池は、NCA正極、LTO負極、そして複合固体電解質から構成されており、独自の加圧溶融含浸法によって作製しました。充放電の過程で、リチウムや遷移金属イオンの信号が可逆的に変化する様子を直接可視化することに成功しました。本研究は、全固体電池内部の反応分布や容量劣化のメカニズムを理解するための新たな可視化手法を示すものです。

権利情報:

キーワード: Operando TOF-SIMS

刊行年月日: 2026-02-13

出版者: American Chemical Society (ACS)

掲載誌:

  • ACS Energy Letters (ISSN: 23808195) vol. 11 issue. 2 p. 1889-1896

研究助成金:

  • Ministry of Education, Culture, Sports, Science and Technology JPMXP0219207397
  • Ministry of Education, Culture, Sports, Science and Technology 24H02205
  • Japan Science and Technology Corporation JPMJGX23S2
  • Japan Science and Technology Corporation JPMJPF2016

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1021/acsenergylett.5c03610

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更新時刻: 2026-02-26 16:30:06 +0900

MDRでの公開時刻: 2026-02-26 13:47:41 +0900

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