Download all files (1.58 MB)

Collection

Citation

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.

Rights:

• In Copyright
  

Keyword: reference-free quantification, NMF, pyrolysis mass spectrometry, nonlinear spectral analysis, compositional analysis for interactive systems

Date published: 2024-09-13

Publisher: Royal Society of Chemistry (RSC)

Journal:

• The Analyst (ISSN: 00032654) vol. 149 p. 5320-5328

Funding:

• Japan Society for the Promotion of Science JP24K08520 (ポリマーシークエンサーを基軸とした配列工学の確立)

Manuscript type: Author's version (Accepted manuscript)

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

First published URL: https://doi.org/10.1039/d4an00961d

Related item:

Other identifier(s):

Contact agent:

Updated at: 2025-09-13 08:30:35 +0900

Published on MDR: 2025-09-13 08:17:22 +0900