Identification of Phosphatidylcholine Isomers in Imaging Mass Spectrometry Using Gas-Phase Charge Inversion Ion/Ion Reactions

Specker, Jonathan T.; Orden, Steven L. Van; Ridgeway, Mark E.; Prentice, Boone M.

doi:10.1021/acs.analchem.0c02350

Cited by 36 publications

(65 citation statements)

References 75 publications

(140 reference statements)

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“…The ESI is a “soft” ionisation method that is suitable for the analysis of polar compounds and thermally unstable substances. Given the rapid development, the ESI can be combined with liquid phase separation equipment at various flow rates [ 24 ]. Phosphatidylcholine has a high sensitivity to ESI [ 25 ] and can be arranged into liposomes to amplify the signal of the measured substance.…”

Section: Resultsmentioning

confidence: 99%

Single-Molecule Detection of Nucleic Acids via Liposome Signal Amplification in Mass Spectrometry

Lin

Zhao

et al. 2022

Sensors

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A single-molecule detection method was developed for nucleic acids based on mass spectrometry counting single liposome particles. Before the appearance of symptoms, a negligible amount of nucleic acids and biomarkers for the clinical diagnosis of the disease were already present. However, it is difficult to detect extremely low concentrations of nucleic acids using the current methods. Hence, the establishment of an ultra-sensitive nucleic acid detection technique is urgently needed. Herein, magnetic beads were used to capture target nucleic acids, and liposome particles were employed as mass tags for single-particle measurements. Liposomes were released from magnetic beads via photocatalytic cleavage. Hence, one DNA molecule corresponded to one liposome particle, which could be counted using mass spectrometric measurement. The ultrasensitive detection of DNA (10–18 M) was achieved using this method.

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Section: Resultsmentioning

confidence: 99%

Single-Molecule Detection of Nucleic Acids via Liposome Signal Amplification in Mass Spectrometry

Lin

Zhao

et al. 2022

Sensors

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“…The reaction between high-energy photons and lipid ions released from tissue allowed for a characteristic dissociation and localization of structural isomeric features. Charge inversion of lipid cations with ion-ion reactions in the gas phase revealed structural information that would not have been observed by dissociation of the original cation (Specker et al, 2020).…”

Section: Lipidomicsmentioning

confidence: 99%

“…This method identified notable changes in abundance of PC isomers between white and gray matter of mouse and human brain tissues and between cancerous and healthy portions of human lymph node. Recently, ion-ion reactions were applied to image PC structures in rat brain by gasphase charge inversion (Specker et al, 2020). Briefly, the mass analyzer was modified to trap lipid cations generated from the tissue surface by MALDI within the collision cell.…”

Section: Unsaturated Systems (Alkenes)mentioning

confidence: 99%

On‐tissue chemical derivatization in mass spectrometry imaging

Harkin

Smith

Cruickshank

et al. 2021

Mass Spectrometry Reviews

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Mass spectrometry imaging (MSI) combines molecular and spatial information in a valuable tool for a wide range of applications. Matrix-assisted laser desorption/ ionization (MALDI) is at the forefront of MSI ionization due to its wide availability and increasing improvement in spatial resolution and analysis speed.However, ionization suppression, low concentrations, and endogenous and methodological interferences cause visualization problems for certain molecules. Chemical derivatization (CD) has proven a viable solution to these issues when applied in mass spectrometry platforms. Chemical tagging of target analytes with larger, precharged moieties aids ionization efficiency and removes analytes from areas of potential isobaric interferences. Here, we address the application of CD on tissue samples for MSI analysis, termed on-tissue chemical derivatization (OTCD). MALDI MSI will remain the focus platform due to its popularity, however, alternative ionization techniques such as liquid extraction surface analysis and desorption electrospray ionization will also be recognized. OTCD reagent selection, application, and optimization methods will be discussed in detail. MSI with OTCD is a powerful tool to study the spatial distribution of poorly ionizable molecules within tissues. Most importantly, the use of OTCD−MSI facilitates the analysis of previously inaccessible biologically relevant molecules through the adaptation of existing CD methods. Though further experimental optimization steps are necessary, the benefits of this technique are extensive.

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“…Bednařík et al used on-tissue PB derivatization followed by MALDI-MS 2 I with a specialized postionization setup to distinguish PC/PS DB positions in rat brain [155]. Also on-tissue epoxidation [156], on-tissue ozonolysis [126], OzID [157], ion/ion reactions [158], and EID [159] have been utilized to reveal different lipid isomers and track their distributions in tissues. Most of these reports demonstrate the performance characteristics of the developed bioanalytic tools but Young et al used MALDI-OzID-MSI to show that the metabolic demand of cancer infection can alter canonical FA and GP formation, thereby creating lipids with unusual DB positions [160].…”

Section: Mass Spectrometry Imaging and Structure Annotationsmentioning

confidence: 99%

Advanced tandem mass spectrometry in metabolomics and lipidomics—methods and applications

Heiles

2021

Anal Bioanal Chem

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Metabolomics and lipidomics are new drivers of the omics era as molecular signatures and selected analytes allow phenotypic characterization and serve as biomarkers, respectively. The growing capabilities of untargeted and targeted workflows, which primarily rely on mass spectrometric platforms, enable extensive charting or identification of bioactive metabolites and lipids. Structural annotation of these compounds is key in order to link specific molecular entities to defined biochemical functions or phenotypes. Tandem mass spectrometry (MS), first and foremost collision-induced dissociation (CID), is the method of choice to unveil structural details of metabolites and lipids. But CID fragment ions are often not sufficient to fully characterize analytes. Therefore, recent years have seen a surge in alternative tandem MS methodologies that aim to offer full structural characterization of metabolites and lipids. In this article, principles, capabilities, drawbacks, and first applications of these “advanced tandem mass spectrometry” strategies will be critically reviewed. This includes tandem MS methods that are based on electrons, photons, and ion/molecule, as well as ion/ion reactions, combining tandem MS with concepts from optical spectroscopy and making use of derivatization strategies. In the final sections of this review, the first applications of these methodologies in combination with liquid chromatography or mass spectrometry imaging are highlighted and future perspectives for research in metabolomics and lipidomics are discussed. Graphical abstract

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Identification of Phosphatidylcholine Isomers in Imaging Mass Spectrometry Using Gas-Phase Charge Inversion Ion/Ion Reactions

Cited by 36 publications

References 75 publications

Single-Molecule Detection of Nucleic Acids via Liposome Signal Amplification in Mass Spectrometry

Single-Molecule Detection of Nucleic Acids via Liposome Signal Amplification in Mass Spectrometry

On‐tissue chemical derivatization in mass spectrometry imaging

Advanced tandem mass spectrometry in metabolomics and lipidomics—methods and applications

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