Review on the manuscript "Molecular Characterization of Alkyl Nitrates in Atmospheric Aerosols by Ion Mobility Mass Spectrometry” by Xuan Zhang et al.

Abstract. We demonstrate the capability of the ion mobility mass spectrometry (IMS-MS) for molecular characterization of reactive and short-lived alkyl nitrates (ANs) in atmospheric aerosols. We show significantly enhanced sensitivity towards the intact molecules of ANs by ultimately 2 orders of magnitude with the addition of inorganic anions such as chloride and nitrate to the negative electrospray to promote the ion adduct formation. This approach enables the measurement of ANs that have a low tendency to form molecular ions on their own with an improved limit of detection in the range of 0.1 to 4.3 µM. Molecular identities of the ANs are well constrained by the developed correlation between the collision cross section and mass-to-charge ratio, which provides a two-dimensional separation of the -ONO2-containing compounds on the basis of their molecular size and geometry. Structural information of the nitrate molecules is further probed by the identification of characteristic fragments produced from the collision-induced dissociation of parent AN adducts. Application of the IMS-MS technique is exemplified by the identification of hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.

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Molecular Characterization of Alkyl Nitrates in Atmospheric Aerosols by Ion Mobility Mass Spectrometry

10.5194/amt-2019-184 ◽

2019 ◽

Cited By ~ 1

Author(s):

Xuan Zhang ◽

Haofei Zhang ◽

Wen Xu ◽

Geoffrey S. Tyndall ◽

John J. Orlando ◽

...

Keyword(s):

Mass Spectrometry ◽

Molecular Characterization ◽

Ion Mobility ◽

Atmospheric Aerosols ◽

Molecular Ions ◽

Charge Ratio ◽

Ion Mobility Mass Spectrometry ◽

Alkyl Nitrates ◽

Enhanced Production

Abstract. We demonstrate the capability of the Ion Mobility Mass Spectrometry (IMS-MS) for molecular characterization of reactive and short-lived alkyl nitrates (ANs) in atmospheric aerosols. We show significantly enhanced production of ion adducts from a selection of alkyl nitrates by clustering with inorganic anions such as chloride and nitrate during negative electrospray, a special chemical ionization mechanism in the condensed phase. This approach enables the detection of ANs that have low tendency to form molecular ions on their own by electrospray ionization. Molecular identity of each AN adduct is well constrained by the developed collision cross section vs. mass to charge ratio correlation, which provides a two-dimensional separation of the –ONO2 containing compounds on the basis of their molecular size and geometry. Structural information of AN molecules is further probed by the identification of characteristic fragments produced from the collision induced dissociation of parent AN adducts. Application of the IMS-MS technique is exemplified by the identification of hydroxy nitrates in secondary organic aerosols produced from isoprene photochemistry.

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Ion Mobility–Mass Spectrometry for Bioanalysis

Separations ◽

10.3390/separations8030033 ◽

2021 ◽

Vol 8 (3) ◽

pp. 33

Author(s):

Xavier Garcia ◽

Maria del Mar Sabaté ◽

Jorge Aubets ◽

Josep Maria Jansat ◽

Sonia Sentellas

Keyword(s):

Mass Spectrometry ◽

Liquid Chromatography ◽

Ion Mobility Spectrometry ◽

Ion Mobility ◽

Biological Samples ◽

Ion Mobility Mass Spectrometry ◽

Exogenous Compounds ◽

Analytical Separation

This paper aims to cover the main strategies based on ion mobility spectrometry (IMS) for the analysis of biological samples. The determination of endogenous and exogenous compounds in such samples is important for the understanding of the health status of individuals. For this reason, the development of new approaches that can be complementary to the ones already established (mainly based on liquid chromatography coupled to mass spectrometry) is welcomed. In this regard, ion mobility spectrometry has appeared in the analytical scenario as a powerful technique for the separation and characterization of compounds based on their mobility. IMS has been used in several areas taking advantage of its orthogonality with other analytical separation techniques, such as liquid chromatography, gas chromatography, capillary electrophoresis, or supercritical fluid chromatography. Bioanalysis is not one of the areas where IMS has been more extensively applied. However, over the last years, the interest in using this approach for the analysis of biological samples has clearly increased. This paper introduces the reader to the principles controlling the separation in IMS and reviews recent applications using this technique in the field of bioanalysis.

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Recent advances in ion mobility–mass spectrometry for improved structural characterization of glycans and glycoconjugates

Current Opinion in Chemical Biology ◽

10.1016/j.cbpa.2017.10.007 ◽

2018 ◽

Vol 42 ◽

pp. 1-8 ◽

Cited By ~ 28

Author(s):

Zhengwei Chen ◽

Matthew S Glover ◽

Lingjun Li

Keyword(s):

Mass Spectrometry ◽

Structural Characterization ◽

Ion Mobility ◽

Ion Mobility Mass Spectrometry ◽

Recent Advances

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Structural Characterization of Methylenedianiline Regioisomers by Ion Mobility-Mass Spectrometry and Tandem Mass Spectrometry. 4. 3-Ring and 4-Ring Isomers

Analytical Chemistry ◽

10.1021/acs.analchem.8b04103 ◽

2018 ◽

Vol 90 (24) ◽

pp. 14453-14461 ◽

Cited By ~ 1

Author(s):

Tiffany M. Crescentini ◽

Sarah M. Stow ◽

Jay G. Forsythe ◽

Jody C. May ◽

John A. McLean ◽

...

Keyword(s):

Mass Spectrometry ◽

Tandem Mass Spectrometry ◽

Structural Characterization ◽

Ion Mobility ◽

Ion Mobility Mass Spectrometry ◽

Tandem Mass

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A Novel Approach to Characterize the Lipidome of Marine Archaeon Nitrosopumilus maritimus by Ion Mobility Mass Spectrometry

Frontiers in Microbiology ◽

10.3389/fmicb.2021.735878 ◽

2021 ◽

Vol 12 ◽

Author(s):

Kai P. Law ◽

Wei He ◽

Jianchang Tao ◽

Chuanlun Zhang

Keyword(s):

Mass Spectrometry ◽

Cross Sections ◽

Ion Mobility ◽

Resolving Power ◽

Ion Mobility Mass Spectrometry ◽

Ion Chemistry ◽

Lipid Species ◽

Mobility System ◽

Archaeal Lipids

Archaea are differentiated from the other two domains of life by their biomolecular characteristics. One such characteristic is the unique structure and composition of their lipids. Characterization of the whole set of lipids in a biological system (the lipidome) remains technologically challenging. This is because the lipidome is innately complex, and not all lipid species are extractable, separable, or ionizable by a single analytical method. Furthermore, lipids are structurally and chemically diverse. Many lipids are isobaric or isomeric and often indistinguishable by the measurement of mass or even their fragmentation spectra. Here we developed a novel analytical protocol based on liquid chromatography ion mobility mass spectrometry to enhance the coverage of the lipidome and characterize the conformations of archaeal lipids by their collision cross-sections (CCSs). The measurements of ion mobility revealed the gas-phase ion chemistry of representative archaeal lipids and provided further insights into their attributions to the adaptability of archaea to environmental stresses. A comprehensive characterization of the lipidome of mesophilic marine thaumarchaeon, Nitrosopumilus maritimus (strain SCM1) revealed potentially an unreported phosphate- and sulfate-containing lipid candidate by negative ionization analysis. It was the first time that experimentally derived CCS values of archaeal lipids were reported. Discrimination of crenarchaeol and its proposed stereoisomer was, however, not achieved with the resolving power of the SYNAPT G2 ion mobility system, and a high-resolution ion mobility system may be required for future work. Structural and spectral libraries of archaeal lipids were constructed in non-vendor-specific formats and are being made available to the community to promote research of Archaea by lipidomics.

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