Automated peak width measurements for targeted analysis of ion mobility unresolved species

Brantley, Matthew R.; Pettit, Michael E.; Harper, Brett; Brown, Brooke A.; Solouki, Touradj

doi:10.1016/j.aca.2016.08.019

Cited by 7 publications

(2 citation statements)

References 71 publications

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“…First, tandem mass spectrometry (MS/MS) by collision-induced dissociation (CID) enables the identification of the molecular core of the compounds. ,− Second, the ion mobility separation enables the separation of the isomers. − Ion mobility spectrometry (IMS) ,− is a technique for separating ions in a gas phase according to their effective ion mobility. − With the use of molecules with a known collision cross section (CCS) as calibrants, the CCS values are determined acting as a direct descriptor of the molecular structure of the ion. The apex of the ion mobility signal is related to the average CCS value of the isomeric mixture, whereas the full width at half maximum (fwhm) is related to the isomeric complexity/diversity. ,,,− In combination with the knowledge of the molecular core, isomeric derivatives can be studied. In the context of petroleum analysis, this is typically related to different patterns in alkylation (length and position) …”

Section: Introductionmentioning

confidence: 99%

“…38−41 With the use of molecules with a known collision cross section (CCS) as calibrants, the CCS values are determined acting as a direct descriptor of the molecular structure of the ion. The apex of the ion mobility signal is related to the average CCS value of the isomeric mixture, whereas the full width at half maximum (fwhm) 42 is related to the isomeric complexity/ diversity. 38,39,41,43−45 In combination with the knowledge of the molecular core, isomeric derivatives can be studied.…”

Section: ■ Introductionmentioning

confidence: 99%

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Structural Analysis of Neutral Nitrogen Compounds Refractory to the Hydrodenitrogenation Process of Heavy Oil Fractions by High-Resolution Tandem Mass Spectrometry and Ion Mobility–Mass Spectrometry

et al. 2020

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This study aims to identify and characterize compounds refractory to hydrodenitrogenation (HDN). The efficiency of a vacuum hydrocracking unit in removing nitrogen-containing compounds to produce a low-nitrogen-content effluent is examined. Molecular, structural, and compositional knowledge is a requisite for the optimization development of the hydrotreatment step processing unit because changes in the chemical composition of petroleum have a direct impact on physical properties and, thus, overall vacuum gas oil (VGO) upgrading processes. Two samples, a VGO and a effluent obtained after the HDN process containing 10 wppm of N, were analyzed by negative-mode electrospray ionization ultra-high-resolution tandem mass spectrometry (ESI–FT-ICR) and ion mobility spectrometry–mass spectrometry (IMS–MS). FT-ICR mass spectrometry provides ultrahigh mass resolving power to separate and characterize compounds in the highly complex petroleum samples. The fragments generated by MS/MS of selected N1 refractory compounds were used for structural elucidation. Species with a double bond equivalent of 10 and 13, which proved to be highly refractory, were analyzed in more detail. On the other hand, the TWIMS–TOF MS measurements enabled the entire ion mobility analysis of refractory species to hydrotreatment processes. The MS/MS spectra revealed a specific pattern allowing for the identification of the molecular nucleus. Furthermore, it allowed for the understanding of the fragmentation pathways: loss of alkyl chains in the first step and opening and rearrangement of the nuclei after that. Ion mobility separation, in combination with MS/MS, allowed for the identification of the different conformations and the revealment of the typical fragments of these molecular nuclei. In particular, the ion mobility peak width indicates isomeric diversity and collision cross section (CCS) determination and provides structural information. The IMS analysis of the identified refractory precursor shows the evolution of its compounds at different processing stages and indicates that some families and structural conformations of N1 species are more resistant to hydrotreatment. Isomers presenting low CCS values in negative mode are more resistant to HDN processes. The combination of TWIMS–TOF MS and ultra-high-resolution mass spectrometry opens exciting and promising prospects for structural determination of complex mixtures, in particular, problematic compounds in petroleum refining processes.

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Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Structural Analysis of Neutral Nitrogen Compounds Refractory to the Hydrodenitrogenation Process of Heavy Oil Fractions by High-Resolution Tandem Mass Spectrometry and Ion Mobility–Mass Spectrometry

et al. 2020

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Signatures of Mechanically Interlocked Topology of Lasso Peptides by Ion Mobility–Mass Spectrometry: Lessons from a Collection of Representatives

Fouque

Lavanant

Zirah

et al. 2016

J. Am. Soc. Mass Spectrom.

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Lasso peptides are characterized by a mechanically interlocked structure, where the C-terminal tail of the peptide is threaded and trapped within an N-terminal macrolactam ring. Their compact and stable structures have a significant impact on their biological and physical properties and make them highly interesting for drug development. Ion mobility - mass spectrometry (IM-MS) has shown to be effective to discriminate the lasso topology from their corresponding branched-cyclic topoisomers in which the C-terminal tail is unthreaded. In fact, previous comparison of the IM-MS data of the two topologies has yielded three trends that allow differentiation of the lasso fold from the branched-cyclic structure: (1) the low abundance of highly charged ions, (2) the low change in collision cross sections (CCS) with increasing charge state and (3) a narrow ion mobility peak width. In this study, a three-dimensional plot was generated using three indicators based on these three trends: (1) mean charge divided by mass (ζ), (2) relative range of CCS covered by all protonated molecules (ΔΩ/Ω) and (3) mean ion mobility peak width (δΩ). The data were first collected on a set of twenty one lasso peptides and eight branched-cyclic peptides. The indicators were obtained also for eight variants of the well-known lasso peptide MccJ25 obtained by site-directed mutagenesis and further extended to five linear peptides, two macrocyclic peptides and one disulfide constrained peptide. In all cases, a clear clustering was observed between constrained and unconstrained structures, thus providing a new strategy to discriminate mechanically interlocked topologies. Graphical Abstract ᅟ.

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Effective Ion Mobility Peak Width as a New Isomeric Descriptor for the Untargeted Analysis of Complex Mixtures Using Ion Mobility-Mass Spectrometry

Farenc

Paupy

Marceau

et al. 2017

J. Am. Soc. Mass Spectrom.

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Ion mobility coupled with mass spectrometry was proven to be an efficient way to characterize complex mixtures such as petroleum samples. However, the identification of isomeric species is difficult owing to the molecular complexity of petroleum and no availability of standard molecules. This paper proposes a new simple indicator to estimate the isomeric content of highly complex mixtures. This indicator is based on the full width at half maximum (FWHM) of the extracted ion mobility peak measured in millisecond or square angstrom that is corrected for instrumental factors such as ion diffusion. This value can be easily obtained without precisely identifying the number of isomeric species under the ion mobility peaks. Considering the Boduszynski model, the ion mobility profile for a particular elemental composition is expected to be a continuum of various isomeric species. The drift time-dependent fragmentation profile was studied and confirmed this hypothesis, a continuous evolution of the fragmentation profile showing that the larger alkyl chain species were detected at higher drift time values. This new indicator was proven to be a fast and efficient method to compare vacuum gas oils for which no difference was found using other analytical techniques. Graphical Abstract ᅟ.

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Automated peak width measurements for targeted analysis of ion mobility unresolved species

Cited by 7 publications

References 71 publications

Structural Analysis of Neutral Nitrogen Compounds Refractory to the Hydrodenitrogenation Process of Heavy Oil Fractions by High-Resolution Tandem Mass Spectrometry and Ion Mobility–Mass Spectrometry

Structural Analysis of Neutral Nitrogen Compounds Refractory to the Hydrodenitrogenation Process of Heavy Oil Fractions by High-Resolution Tandem Mass Spectrometry and Ion Mobility–Mass Spectrometry

Signatures of Mechanically Interlocked Topology of Lasso Peptides by Ion Mobility–Mass Spectrometry: Lessons from a Collection of Representatives

Effective Ion Mobility Peak Width as a New Isomeric Descriptor for the Untargeted Analysis of Complex Mixtures Using Ion Mobility-Mass Spectrometry

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