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

https://mdr.nims.go.jp/datasets/e4ede7e5-db30-4d91-9940-f76f4899ef7f

## File

- [Xing2026_operando-time-of-flight-secondary-ion-mass-spectrometry-visualization-of-reversible-and-irreversible-reactions-in-oxide.pdf](https://mdr.nims.go.jp/filesets/6409fdfa-4ef9-4d09-b0f1-3f21a9dd655a/download) ([Detail](https://mdr.nims.go.jp/filesets/6409fdfa-4ef9-4d09-b0f1-3f21a9dd655a.md))

## Id

e4ede7e5-db30-4d91-9940-f76f4899ef7f

## Local identifier



## Visibility

open_to_public

## State

published

## Created at

2026-02-25T08:30:24.369360Z

## Updated at

2026-02-26T07:30:06.770228Z

## Published at

2026-02-26T04:47:41.632605Z

## Doi



## First published url

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

## Date published

2026-02-13

## Recorded date published

2026-2-13

## Resource type

journal_article

## Manuscript type

vor

## Collection



## Title

- title: Operando Time-of-Flight Secondary Ion Mass Spectrometry Visualization of
    Reversible and Irreversible Reactions in Oxide-Based Solid-State Batteries
  title_type: original
  lang: en

## Description

- description: "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.\r\n\r\n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。"
  description_type: abstract
  lang: und

## Creator

- name: Sihao Xing
  role: author
- name: Gen Hasegawa
  role: author
  orcid: https://orcid.org/0000-0002-9297-6902
- name: Prince Sharma
  role: author
- name: Daisuke Ito
  role: author
  orcid: https://orcid.org/0009-0006-9296-1926
- name: Kazuhiro Kamiguchi
  role: author
- name: Kazunori Takada
  role: author
  orcid: https://orcid.org/0000-0001-7568-1806
- name: Naoaki Kuwata
  role: author
  orcid: https://orcid.org/0000-0002-0736-6967

## Contact agent



## Publisher

organization: American Chemical Society (ACS)

## Managing organization



## Keyword

- subject: Operando TOF-SIMS
  schema: not_defined

## Rights

- identifier: https://creativecommons.org/licenses/by/4.0/

## Other identifier(s)



## Data origin

- data_origin_type: other

## Embargo



## Journal

- title: ACS Energy Letters
  issn: '23808195'
  volume: '11'
  issue: '2'
  start_page: 1889
  end_page: 1896

## Conference



## Related item



## Funding

- identifier: JPMXP0219207397
  funder_name: Ministry of Education, Culture, Sports, Science and Technology
- identifier: 24H02205
  funder_name: Ministry of Education, Culture, Sports, Science and Technology
- identifier: JPMJGX23S2
  funder_name: Japan Science and Technology Corporation
- identifier: JPMJPF2016
  funder_name: Japan Science and Technology Corporation

## Instrument



## Instrument operator



## Instrument managing organization



## Measurement method



## Specimen



## Chemical composition



## Structure for specimen



## Structural feature for specimen



## Specific property for specimen



## Process for specimen treatment



## Computational method



## Energy level/transition state



## Software



## Custom property



## Fileset

- id: 6409fdfa-4ef9-4d09-b0f1-3f21a9dd655a
  filename: Xing2026_operando-time-of-flight-secondary-ion-mass-spectrometry-visualization-of-reversible-and-irreversible-reactions-in-oxide.pdf
  content_type: application/pdf
  size: 6633161
  md5: 41c6aa2c96721a517907437abac5853d

## Thumbnail

fileset_id: 6409fdfa-4ef9-4d09-b0f1-3f21a9dd655a
filename: Xing2026_operando-time-of-flight-secondary-ion-mass-spectrometry-visualization-of-reversible-and-irreversible-reactions-in-oxide.pdf