Permethylation and Metal Adduction: A Toolbox for the Improved Characterization of Glycolipids with Cyclic Ion Mobility Separations Coupled to Mass Spectrometry

Naylor, Cameron N.; Nagy, Gabe

doi:10.1021/acs.analchem.3c03448

Cited by 4 publications

(1 citation statement)

References 53 publications

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“…Specifically, advancements in high‐resolution IMS‐MS platforms (e.g., structures for lossless ion manipulations, SLIM and cyclic IMS, cIMS) have enabled the rapid separation of isomers that were previously intractable with condensed‐phase methods 21,22 . While in certain cases, high‐resolution IMS‐MS separations have remained qualitative in nature, 22–30 our group, among others, has developed calibration strategies for determining rotationally averaged ion‐neutral collision cross section (CCS) values in multipass separations 31–33 . In this work, we set out to develop a cIMS‐MS‐based CCS library of permethylated HMO standards, where their structures are shown with symbolic nomenclature in Figure 1.…”

Section: Introductionmentioning

confidence: 99%

Development of a cyclic ion mobility spectrometry‐mass spectrometry‐based collision cross‐section database of permethylated human milk oligosaccharides

Habibi,

Bradford,

Baird

et al. 2024

J Mass Spectrom

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Human milk oligosaccharides (HMOs) are an important class of biomolecules responsible for the healthy development of the brain‐gut axis of infants. Unfortunately, their accurate characterization is largely precluded due to a variety of reasons – there are over 200 possible HMO structures whereas only 10s of these are available as authentic analytical standards. Furthermore, their isomeric heterogeneity stemming from their many possible glycosidic linkage positions and corresponding α/β anomericities further complicates their analyses. While liquid chromatography coupled to tandem mass spectrometry remains the gold standard for HMO analyses, it often times cannot resolve all possible isomeric species and thus warrants the development of other orthogonal approaches. High‐resolution ion mobility spectrometry coupled to mass spectrometry has emerged as a rapid alternative to condensed‐phase separations but largely has remained limited to qualitative information related to the resolution of isomers. In this work, we have assessed the use of permethylation to improve both the resolution and sensitivity of HMO analyses with cyclic ion mobility separations coupled with mass spectrometry. In addition to this, we have developed the first‐ever high‐resolution collision cross‐section database for permethylated HMOs using our previously established calibration protocol. We envision that this internal reference database generated from high‐resolution cyclic ion mobility spectrometry‐mass spectrometry will greatly aid in the accurate characterization of HMOs and provide a valuable, orthogonal, approach to existing liquid chromatography–tandem mass spectrometry‐based methods.

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Section: Introductionmentioning

confidence: 99%

Development of a cyclic ion mobility spectrometry‐mass spectrometry‐based collision cross‐section database of permethylated human milk oligosaccharides

Habibi,

Bradford,

Baird

et al. 2024

J Mass Spectrom

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Recent advances in high‐resolution traveling wave‐based ion mobility separations coupled to mass spectrometry

Naylor,

Nagy

2024

Mass Spectrometry Reviews

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Recently, ion mobility spectrometry‐mass spectrometry (IMS‐MS) has become more readily incorporated into various omics‐based workflows. These growing applications are due to developments in instrumentation within the last decade that have enabled higher‐resolution ion mobility separations. Two such platforms are the cyclic (cIMS) and structures for lossless ion manipulations (SLIM), both of which use traveling wave ion mobility spectrometry (TWIMS). High‐resolution separations achieved with these techniques stem from the drastically increased pathlengths, on the order of 10 s of meters to >1 km, in both cIMS‐MS and SLIM IMS‐MS, respectively. Herein, we highlight recent developments and advances, for the period 2019–2023, in high‐resolution traveling wave‐based IMS‐MS through instrumentation, calibration strategies, hyphenated techniques, and applications. Specifically, we will discuss applications including CCS calculations in multipass IMS‐MS separations, coupling of IMS‐MS with chromatography, imaging, and cryogenic infrared spectroscopy, and isomeric separations of glycans, lipids, and other small metabolites.

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Multi-Pass Arrival Time Correction in Cyclic Ion Mobility Mass Spectrometry for Imaging and Shotgun Lipidomics

Wisanpitayakorn,

Jariyasopit,

Duangkumpha

et al. 2024

ACS Meas. Sci. Au

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Direct-infusion mass spectrometry (DI-MS) and mass spectrometry imaging (MSI) are powerful techniques for lipidomics research. However, annotating isomeric and isobaric lipids with these methods is challenging due to the absence of chromatographic separation. Recently, cyclic ion mobility mass spectrometry (cIM-MS) has been proposed to overcome this limitation. However, fluctuations in room conditions can affect ion mobility multipass arrival times, potentially reducing annotation confidence. In this study, we developed a multipass arrival time correction method that proved effective across various dates, room temperatures, ion mobility settings, and laboratories using mixtures of reference standards. We observed slight variations in the linear correction lines between lipid and nonlipid molecules, underscoring the importance of choosing appropriate reference molecules. Based on these results, we demonstrated that an accurate multipass arrival time database can be constructed from corrected t 0 and t p for interlaboratory use and can effectively identify isomeric lipids in MSI using only a single measurement. This approach significantly simplifies the identification process compared to determining multipass collision cross-section, which requires multiple measurements that are both sample-and time-intensive for MSI. Additionally, we validated our multipass drift time correction method in shotgun lipidomics analyses of human and mouse serum samples and observed no matrix effect for the analysis. Despite variations in dates, room temperatures, instruments, and ion mobility settings, our approach reduced the mean drift time differences from over 2% to below 0.2%.

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Permethylation and Metal Adduction: A Toolbox for the Improved Characterization of Glycolipids with Cyclic Ion Mobility Separations Coupled to Mass Spectrometry

Cited by 4 publications

References 53 publications

Development of a cyclic ion mobility spectrometry‐mass spectrometry‐based collision cross‐section database of permethylated human milk oligosaccharides

Development of a cyclic ion mobility spectrometry‐mass spectrometry‐based collision cross‐section database of permethylated human milk oligosaccharides

Recent advances in high‐resolution traveling wave‐based ion mobility separations coupled to mass spectrometry

Multi-Pass Arrival Time Correction in Cyclic Ion Mobility Mass Spectrometry for Imaging and Shotgun Lipidomics

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