Characterization of Electrospray Ionization (ESI) Parameters on In-ESI Hydrogen/Deuterium Exchange of Carbohydrate-Metal Ion Adducts

Liyanage, O. Tara; Brantley, Matthew R.; Calixte, Emvia I.; Solouki, Touradj; Shuford, Kevin L.; Gallagher, Elyssia S.

doi:10.1007/s13361-018-2080-1

Characterization of Electrospray Ionization (ESI) Parameters on In-ESI Hydrogen/Deuterium Exchange of Carbohydrate-Metal Ion Adducts

Journal Article · 23 October 2018 · Journal of the American Society for Mass Spectrometry

DOI:https://doi.org/10.1007/s13361-018-2080-1· OSTI ID:1593751

Liyanage, O. Tara ^[1]; Brantley, Matthew R. ^[1]; Calixte, Emvia I. ^[1]; Solouki, Touradj ^[1]; Shuford, Kevin L. ^[1]; ^[1]

Baylor Univ., Waco, TX (United States)

The conformations of glycans are crucial for their biological functions. In-electrospray ionization (ESI) hydrogen/deuterium exchange-mass spectrometry (HDX-MS) is a promising technique for studying carbohydrate conformations since rapidly exchanging functional groups, e.g., hydroxyls, can be labeled on the timeframe of ESI. However, regular application of in-ESI HDX to characterize carbohydrates requires further analysis of the in-ESI HDX methodology. For instance, in this method, HDX occurs concurrently to the analyte transitioning from solution to gas-phase ions. Therefore, there is a possibility of sampling both gas-phase and solution-phase conformations of the analyte. Herein, we differentiate in-ESI HDX of metal-adducted carbohydrates from gas-phase HDX and illustrate that this method analyzes solvated species. We also systematically examine the effects of ESI parameters, including spray solvent composition, auxiliary gas flow rate, sheath gas flow rate, sample infusion rate, sample concentration, and spray voltage, and discuss their effects on in-ESI HDX. Further, we model the structural changes of a trisaccharide, melezitose, and its intramolecular and intermolecular hydrogen bonding in solvents with different compositions of methanol and water. These molecular dynamic simulations support our experimental results and illustrate how an individual ESI parameter can alter the conformations we sample by in-ESI HDX. Overall, this work illustrates how the fundamental processes of ESI alter the magnitude of HDX for carbohydrates and suggest parameters that should be considered and/or optimized prior to performing experiments with this in-ESI HDX technique.

Research Organization:: Baylor Univ., Waco, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Welch Foundation; National Science Foundation (NSF)

DOE Contract Number:: SC0019327; AA-1899; 1455668

OSTI ID:: 1593751

Journal Information:: Journal of the American Society for Mass Spectrometry, Vol. 30, Issue 2; ISSN 1044-0305

Publisher:: American Society for Mass Spectrometry

Country of Publication:: United States

Language:: English

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