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Proteoform Differentiation using Tandem Trapped Ion Mobility, Electron Capture Dissociation, and ToF Mass Spectrometry

التفاصيل البيبلوغرافية
العنوان: Proteoform Differentiation using Tandem Trapped Ion Mobility, Electron Capture Dissociation, and ToF Mass Spectrometry
المؤلفون: Valery G. Voinov, Ole N. Jensen, Frederik H V Holck, Desmond Allen Kaplan, Francisco Fernandez-Lima, Kevin Jeanne Dit Fouque
المصدر: Anal Chem
Jeanne Dit Fouque, K, Kaplan, D, Voinov, V G, Holck, F H V, Jensen, O N & Fernandez-Lima, F 2021, ' Proteoform Differentiation using Tandem Trapped Ion Mobility, Electron Capture Dissociation, and ToF Mass Spectrometry ', Analytical chemistry, vol. 93, no. 27, pp. 9575–9582 . https://doi.org/10.1021/acs.analchem.1c01735
سنة النشر: 2021
مصطلحات موضوعية: Ions, Electron-capture dissociation, Tandem, Ion-mobility spectrometry, Chemistry, 010401 analytical chemistry, Analytical chemistry, Cell Differentiation, Electrons, 010402 general chemistry, Mass spectrometry, 01 natural sciences, Dissociation (chemistry), Mass Spectrometry, Article, 0104 chemical sciences, Analytical Chemistry, Ion, Fragmentation (mass spectrometry), Ion Mobility Spectrometry, Isobaric process
الوصف: Comprehensive characterization of post-translationally modified histone proteoforms is challenging due to their high isobaric and isomeric content. Trapped ion mobility spectrometry (TIMS), implemented on a quadrupole/time-of-flight (Q-ToF) mass spectrometer, has shown great promise in discriminating isomeric complete histone tails. The absence of electron activated dissociation (ExD) in the current platform prevents the comprehensive characterization of unknown histone proteoforms. In the present work, we report for the first time the use of an electromagnetostatic (EMS) cell devised for nonergodic dissociation based on electron capture dissociation (ECD), implemented within a nESI-TIMS-Q-ToF mass spectrometer for the characterization of acetylated (AcK18 and AcK27) and trimethylated (TriMetK4, TriMetK9 and TriMetK27) complete histone tails. The integration of the EMS cell in a TIMS-q-TOF MS permitted fast mobility-selected top-down ECD fragmentation with near 10% efficiency overall. The potential of this coupling was illustrated using isobaric (AcK18/TriMetK4) and isomeric (AcK18/AcK27 and TriMetK4/TriMetK9) binary H3 histone tail mixtures, and the H3.1 TriMetK27 histone tail structural diversity (e.g., three IMS bands atz= 7+). The binary isobaric and isomeric mixtures can be separated in the mobility domain withR IMS> 100 and the nonergodic ECD fragmentation permitted the PTM localization (sequence coverage of ∼86%). Differences in the ECD patterns per mobility band of thez= 7+ H3 TriMetK27 molecular ions suggested that the charge location is responsible for the structural differences observed in the mobility domain. This coupling further enhances the structural toolbox with fast, high resolution mobility separations in tandem with nonergodic fragmentation for effective proteoform differentiation.
تدمد: 1520-6882
URL الوصول: https://explore.openaire.eu/search/publication?articleId=doi_dedup___::686ffdab557f12501aa15bc2e73e58df
https://pubmed.ncbi.nlm.nih.gov/34170114
حقوق: OPEN
رقم الأكسشن: edsair.doi.dedup.....686ffdab557f12501aa15bc2e73e58df
قاعدة البيانات: OpenAIRE
الوصف
تدمد:15206882