# Reference-free quantitative mass spectrometry in the presence of nonlinear distortion caused by <i>in situ</i> chemical reactions among constituents

https://mdr.nims.go.jp/datasets/2c2282ec-a0e6-4b36-98a4-61f58459fdd7

## File

- [mainText_NL-RQMS_revised.pdf](https://mdr.nims.go.jp/filesets/aae11556-9496-430a-9266-2fdf7766b646/download) ([Detail](https://mdr.nims.go.jp/filesets/aae11556-9496-430a-9266-2fdf7766b646.md))
- [SI_NL-RQMS.pdf](https://mdr.nims.go.jp/filesets/32a78177-92be-4373-8cdc-6a4d89411902/download) ([Detail](https://mdr.nims.go.jp/filesets/32a78177-92be-4373-8cdc-6a4d89411902.md))

## Id

2c2282ec-a0e6-4b36-98a4-61f58459fdd7

## Local identifier



## Visibility

open_to_public

## State

published

## Created at

2024-10-21T11:12:05.384204Z

## Updated at

2025-09-12T23:30:35.345482Z

## Published at

2025-09-12T23:17:22.321761Z

## Doi

https://doi.org/10.48505/nims.4879

## First published url

https://doi.org/10.1039/d4an00961d

## Date published

2024-09-13

## Recorded date published

2024-10-21

## Resource type

journal_article

## Manuscript type

accepted_manuscript

## Collection



## Title

- title: Reference-free quantitative mass spectrometry in the presence of nonlinear
    distortion caused by <i>in situ</i> chemical reactions among constituents
  title_type: original
  lang: en

## Description

- description: Materials performance is primarily influenced by chemical composition,
    making compositional analysis (CA) essential in materials science. Traditional
    quantitative mass spectrometry, which deconvolutes analyte spectra into reference
    spectra, struggles with reactive systems where spectral variations occur, such
    as peak shifts and new peak emergences. Additionally, obtaining reference spectra
    for all pure constituents is often impractical. To address these challenges, I
    propose nonlinear reference-free quantitative mass spectrometry (NL-RQMS). This
    method simultaneously determines composition, reference spectra, and nonlinear
    interaction effects directly from a spectral dataset of mixtures, eliminating
    the need for prior reference spectra. In a benchmark test on ternary reactive
    polymers of epoxy and amines, NL-RQMS inferred compositions with an error margin
    of just 3 wt%, significantly outperforming the 6 wt% error margin of linear RQMS.
    The inferred interaction terms clearly indicate in-situ reactions between epoxy
    and amine moieties. This framework enables accurate compositional analysis without
    prior knowledge of the constituents, even in systems with interactive components,
    and holds significant potential for applications such as grading recycled plastics,
    where pristine materials, degradation compounds, and stabilizers interact complexly,
    causing nonlinear spectral distortions.
  description_type: abstract
  lang: und

## Creator

- name: Yusuke Hibi
  role: author
  orcid: https://orcid.org/0000-0003-4006-1070

## Contact agent



## Publisher

organization: Royal Society of Chemistry (RSC)

## Managing organization



## Keyword

- subject: reference-free quantification
  schema: not_defined
- subject: NMF
  schema: not_defined
- subject: pyrolysis mass spectrometry
  schema: not_defined
- subject: nonlinear spectral analysis
  schema: not_defined
- subject: compositional analysis for interactive systems
  schema: not_defined

## Rights

- identifier: http://rightsstatements.org/vocab/InC/1.0/

## Other identifier(s)



## Data origin

- data_origin_type: other

## Embargo

start_date: 2024-09-13
end_date: 2025-09-13

## Journal

- title: The Analyst
  issn: '00032654'
  volume: '149'
  start_page: 5320
  end_page: 5328

## Conference



## Related item



## Funding

- identifier: JP24K08520
  funder_name: Japan Society for the Promotion of Science
  description: ポリマーシークエンサーを基軸とした配列工学の確立

## 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: aae11556-9496-430a-9266-2fdf7766b646
  filename: mainText_NL-RQMS_revised.pdf
  content_type: application/pdf
  size: 946083
  md5: 959a8a6fa7483ff693cc65c74e20873a
- id: 32a78177-92be-4373-8cdc-6a4d89411902
  filename: SI_NL-RQMS.pdf
  content_type: application/pdf
  size: 1064262
  md5: 22a6a72c74699c7339c0af319085165d

## Thumbnail

fileset_id: 32a78177-92be-4373-8cdc-6a4d89411902
filename: SI_NL-RQMS.pdf