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Gas-phase dynamics of collision induced unfolding, collision induced dissociation, and electron transfer dissociation-activated polymer ions

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Abstract
Polymer characterizations are often performed using mass spectrometry (MS). Aside from MS and different tandem MS (MS/MS) techniques, ion mobility-mass spectrometry (IM-MS) has been recently added to the inventory of characterization technique. However, only few studies have focused on the reproducibility and robustness of polymer IM-MS analyses. Here, we perform collisional and electron-mediated activation of polymer ions before measuring IM drift times, collision cross-sections (CCS), or reduced ion mobilities (K-0). The resulting IM behavior of different activated product ions is then compared to non-activated native intact polymer ions. First, we analyzed collision induced unfolding (CIU) of precursor ions to test the robustness of polymer ion shapes. Then, we focused on fragmentation product ions to test for shape retentions from the precursor ions: cation ejection species (CES) and product ions with m/z and charge state values identical to native intact polymer ions. The CES species are formed using both collision induced dissociation (CID) and electron transfer dissociation (ETD, formally ETnoD) experiments. Only small drift time, CCS, or K-0 deviations between the activated/formed ions are observed compared to the native intact polymer ions. The polymer ion shapes seem to depend solely on their mass and charge state. The experiments were performed on three synthetic homopolymers: poly(ethoxy phosphate) (PEtP), poly(2-n-propyl-2-oxazoline) (Pn-PrOx), and poly(ethylene oxide) (PEO). These results confirm the robustness of polymer ion CCSs for IM calibration, especially singly charged polymer ions. The results are also discussed in the context of polymer analyses, CCS predictions, and probing ion-drift gas interaction potentials.
Keywords
MOBILITY-MASS-SPECTROMETRY, CYTOCHROME-C IONS, CAPTURE-DISSOCIATION, BLOCK-COPOLYMERS, CROSS-SECTIONS, CONFORMATIONS, FRAGMENTATION, POLYALANINE, IONIZATION, ENERGY, Collision induced unfolding, CIU, Collision induced dissociation, CID, Electron transfer dissociation, ETD, Synthetic polymers, Ion mobility, calibration

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MLA
Haler, Jean RN et al. “Gas-phase Dynamics of Collision Induced Unfolding, Collision Induced Dissociation, and Electron Transfer Dissociation-activated Polymer Ions.” JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY 30.4 (2019): 563–572. Print.
APA
Haler, J. R., Massonnet, P., Far, J., Retamero De La Rosa, V., Lecomte, P., Hoogenboom, R., Jerome, C., et al. (2019). Gas-phase dynamics of collision induced unfolding, collision induced dissociation, and electron transfer dissociation-activated polymer ions. JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY, 30(4), 563–572.
Chicago author-date
Haler, Jean RN, Philippe Massonnet, Johann Far, Victor Retamero De La Rosa, Philippe Lecomte, Richard Hoogenboom, Christine Jerome, and Edwin De Pauw. 2019. “Gas-phase Dynamics of Collision Induced Unfolding, Collision Induced Dissociation, and Electron Transfer Dissociation-activated Polymer Ions.” Journal of the American Society for Mass Spectrometry 30 (4): 563–572.
Chicago author-date (all authors)
Haler, Jean RN, Philippe Massonnet, Johann Far, Victor Retamero De La Rosa, Philippe Lecomte, Richard Hoogenboom, Christine Jerome, and Edwin De Pauw. 2019. “Gas-phase Dynamics of Collision Induced Unfolding, Collision Induced Dissociation, and Electron Transfer Dissociation-activated Polymer Ions.” Journal of the American Society for Mass Spectrometry 30 (4): 563–572.
Vancouver
1.
Haler JR, Massonnet P, Far J, Retamero De La Rosa V, Lecomte P, Hoogenboom R, et al. Gas-phase dynamics of collision induced unfolding, collision induced dissociation, and electron transfer dissociation-activated polymer ions. JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY. 2019;30(4):563–72.
IEEE
[1]
J. R. Haler et al., “Gas-phase dynamics of collision induced unfolding, collision induced dissociation, and electron transfer dissociation-activated polymer ions,” JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY, vol. 30, no. 4, pp. 563–572, 2019.
@article{8616607,
  abstract     = {Polymer characterizations are often performed using mass spectrometry (MS). Aside from MS and different tandem MS (MS/MS) techniques, ion mobility-mass spectrometry (IM-MS) has been recently added to the inventory of characterization technique. However, only few studies have focused on the reproducibility and robustness of polymer IM-MS analyses. Here, we perform collisional and electron-mediated activation of polymer ions before measuring IM drift times, collision cross-sections (CCS), or reduced ion mobilities (K-0). The resulting IM behavior of different activated product ions is then compared to non-activated native intact polymer ions. First, we analyzed collision induced unfolding (CIU) of precursor ions to test the robustness of polymer ion shapes. Then, we focused on fragmentation product ions to test for shape retentions from the precursor ions: cation ejection species (CES) and product ions with m/z and charge state values identical to native intact polymer ions. The CES species are formed using both collision induced dissociation (CID) and electron transfer dissociation (ETD, formally ETnoD) experiments. Only small drift time, CCS, or K-0 deviations between the activated/formed ions are observed compared to the native intact polymer ions. The polymer ion shapes seem to depend solely on their mass and charge state. The experiments were performed on three synthetic homopolymers: poly(ethoxy phosphate) (PEtP), poly(2-n-propyl-2-oxazoline) (Pn-PrOx), and poly(ethylene oxide) (PEO). These results confirm the robustness of polymer ion CCSs for IM calibration, especially singly charged polymer ions. The results are also discussed in the context of polymer analyses, CCS predictions, and probing ion-drift gas interaction potentials.},
  author       = {Haler, Jean RN and Massonnet, Philippe and Far, Johann and Retamero De La Rosa, Victor and Lecomte, Philippe and Hoogenboom, Richard and Jerome, Christine and De Pauw, Edwin},
  issn         = {1044-0305},
  journal      = {JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY},
  keywords     = {MOBILITY-MASS-SPECTROMETRY,CYTOCHROME-C IONS,CAPTURE-DISSOCIATION,BLOCK-COPOLYMERS,CROSS-SECTIONS,CONFORMATIONS,FRAGMENTATION,POLYALANINE,IONIZATION,ENERGY,Collision induced unfolding,CIU,Collision induced dissociation,CID,Electron transfer dissociation,ETD,Synthetic polymers,Ion mobility,calibration},
  language     = {eng},
  number       = {4},
  pages        = {563--572},
  title        = {Gas-phase dynamics of collision induced unfolding, collision induced dissociation, and electron transfer dissociation-activated polymer ions},
  url          = {http://dx.doi.org/10.1007/s13361-018-2115-7},
  volume       = {30},
  year         = {2019},
}

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