Identification of Isomeric N-glycans by Conformer Distribution Fingerprinting using Ion Mobility-Mass Spectrometry

Javier Sastre Toraño; Oier Aizpurua-Olaizola; Na Wei; Tiehai Li; Luca Unione; Gonzalo Jiménez-Osés; Francisco Corzana; Victor J Somovilla; Juan M Falcon-Perez; Geert-Jan Boons

doi:10.1002/chem.202004522

Identification of Isomeric N-glycans by Conformer Distribution Fingerprinting using Ion Mobility-Mass Spectrometry

Javier Sastre Toraño, Oier Aizpurua-Olaizola, Na Wei, Tiehai Li, Luca Unione, Gonzalo Jiménez-Osés, Francisco Corzana, Victor J Somovilla, Juan M Falcon-Perez, Geert-Jan Boons

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Glycans possess unparalleled structural complexity arising from chemically similar monosaccharide building blocks, configurations of anomeric linkages and different branching patterns, potentially giving rise to many isomers. This level of complexity is one of the main reasons that identification of exact glycan structures in biological samples still lags behind that of other biomolecules. Here, we introduce a methodology to identify isomeric N-glycans by determining gas phase conformer distributions (CDs) by measuring arrival time distributions (ATDs) using drift-tube ion mobility spectrometry-mass spectrometry . Key to the approach is the use of a range of well-defined synthetic glycans that made it possible to investigate conformer distributions in the gas phase of isomeric glycans in a systematic manner. In addition, we have computed CD fingerprints by molecular dynamics (MD) simulation, which compared well with experimentally determined CDs. It supports that ATDs resemble conformational populations in the gas phase and offer the prospect that such an approach can contribute to generating a library of CCS distributions (CCSDs) for structure identification.

Original language	English
Pages (from-to)	2149-2154
Number of pages	6
Journal	Chemistry-A European Journal
Volume	27
Issue number	6
Early online date	13 Oct 2020
DOIs	https://doi.org/10.1002/chem.202004522
Publication status	Published - 26 Jan 2021

Bibliographical note

Funding Information:
This project was supported by the Basque Government (postdoctoral fellowship to O.A.O.), EU Commission (Marie Skłodowska‐Curie 749996 to V.J.S.), Spanish Ministry of Science and Innovation (MCI) (FEDER funds RTI2018‐099592‐B‐C21 to F.C and RTI2018‐099592‐B‐C22 to G.J.O, the Human Frontier Science Program (postdoctoral fellowship LT000747/208‐C to L.U.) and the National Institute of Standard and Technology (NIST) (60NANB16D265 to G.J.B.).

Funding Information:
This project was supported by the Basque Government (postdoctoral fellowship to O.A.O.), EU Commission (Marie Sk?odowska-Curie 749996 to V.J.S.), Spanish Ministry of Science and Innovation (MCI) (FEDER funds RTI2018-099592-B-C21 to F.C and RTI2018-099592-B-C22 to G.J.O, the Human Frontier Science Program (postdoctoral fellowship LT000747/208-C to L.U.) and the National Institute of Standard and Technology (NIST) (60NANB16D265 to G.J.B.).

Publisher Copyright:
© 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH

Keywords

carbohydrates
chemo-enzymatic synthesis
conformations
ion mobility spectrometry
mass spectrometry
molecular dynamics

Access to Document

10.1002/chem.202004522Licence: CC BY-NC

chem.202004522Final published version, 1.25 MBLicence: CC BY-NC

Cite this

Sastre Toraño, J., Aizpurua-Olaizola, O., Wei, N., Li, T., Unione, L., Jiménez-Osés, G., Corzana, F., Somovilla, V. J., Falcon-Perez, J. M., & Boons, G.-J. (2021). Identification of Isomeric N-glycans by Conformer Distribution Fingerprinting using Ion Mobility-Mass Spectrometry. Chemistry-A European Journal, 27(6), 2149-2154. https://doi.org/10.1002/chem.202004522

@article{9f07d5a0fad04778a8290d285480b6a1,

title = "Identification of Isomeric N-glycans by Conformer Distribution Fingerprinting using Ion Mobility-Mass Spectrometry",

abstract = "Glycans possess unparalleled structural complexity arising from chemically similar monosaccharide building blocks, configurations of anomeric linkages and different branching patterns, potentially giving rise to many isomers. This level of complexity is one of the main reasons that identification of exact glycan structures in biological samples still lags behind that of other biomolecules. Here, we introduce a methodology to identify isomeric N-glycans by determining gas phase conformer distributions (CDs) by measuring arrival time distributions (ATDs) using drift-tube ion mobility spectrometry-mass spectrometry . Key to the approach is the use of a range of well-defined synthetic glycans that made it possible to investigate conformer distributions in the gas phase of isomeric glycans in a systematic manner. In addition, we have computed CD fingerprints by molecular dynamics (MD) simulation, which compared well with experimentally determined CDs. It supports that ATDs resemble conformational populations in the gas phase and offer the prospect that such an approach can contribute to generating a library of CCS distributions (CCSDs) for structure identification.",

keywords = "carbohydrates, chemo-enzymatic synthesis, conformations, ion mobility spectrometry, mass spectrometry, molecular dynamics",

author = "\{Sastre Tora{\~n}o\}, Javier and Oier Aizpurua-Olaizola and Na Wei and Tiehai Li and Luca Unione and Gonzalo Jim{\'e}nez-Os{\'e}s and Francisco Corzana and Somovilla, \{Victor J\} and Falcon-Perez, \{Juan M\} and Geert-Jan Boons",

note = "Funding Information: This project was supported by the Basque Government (postdoctoral fellowship to O.A.O.), EU Commission (Marie Sk{\l}odowska‐Curie 749996 to V.J.S.), Spanish Ministry of Science and Innovation (MCI) (FEDER funds RTI2018‐099592‐B‐C21 to F.C and RTI2018‐099592‐B‐C22 to G.J.O, the Human Frontier Science Program (postdoctoral fellowship LT000747/208‐C to L.U.) and the National Institute of Standard and Technology (NIST) (60NANB16D265 to G.J.B.). Funding Information: This project was supported by the Basque Government (postdoctoral fellowship to O.A.O.), EU Commission (Marie Sk?odowska-Curie 749996 to V.J.S.), Spanish Ministry of Science and Innovation (MCI) (FEDER funds RTI2018-099592-B-C21 to F.C and RTI2018-099592-B-C22 to G.J.O, the Human Frontier Science Program (postdoctoral fellowship LT000747/208-C to L.U.) and the National Institute of Standard and Technology (NIST) (60NANB16D265 to G.J.B.). Publisher Copyright: {\textcopyright} 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH",

year = "2021",

month = jan,

day = "26",

doi = "10.1002/chem.202004522",

language = "English",

volume = "27",

pages = "2149--2154",

journal = "Chemistry-A European Journal",

issn = "0947-6539",

publisher = "John Wiley and Sons Inc.",

number = "6",

}

TY - JOUR

T1 - Identification of Isomeric N-glycans by Conformer Distribution Fingerprinting using Ion Mobility-Mass Spectrometry

AU - Sastre Toraño, Javier

AU - Aizpurua-Olaizola, Oier

AU - Wei, Na

AU - Li, Tiehai

AU - Unione, Luca

AU - Jiménez-Osés, Gonzalo

AU - Corzana, Francisco

AU - Somovilla, Victor J

AU - Falcon-Perez, Juan M

AU - Boons, Geert-Jan

N1 - Funding Information: This project was supported by the Basque Government (postdoctoral fellowship to O.A.O.), EU Commission (Marie Skłodowska‐Curie 749996 to V.J.S.), Spanish Ministry of Science and Innovation (MCI) (FEDER funds RTI2018‐099592‐B‐C21 to F.C and RTI2018‐099592‐B‐C22 to G.J.O, the Human Frontier Science Program (postdoctoral fellowship LT000747/208‐C to L.U.) and the National Institute of Standard and Technology (NIST) (60NANB16D265 to G.J.B.). Funding Information: This project was supported by the Basque Government (postdoctoral fellowship to O.A.O.), EU Commission (Marie Sk?odowska-Curie 749996 to V.J.S.), Spanish Ministry of Science and Innovation (MCI) (FEDER funds RTI2018-099592-B-C21 to F.C and RTI2018-099592-B-C22 to G.J.O, the Human Frontier Science Program (postdoctoral fellowship LT000747/208-C to L.U.) and the National Institute of Standard and Technology (NIST) (60NANB16D265 to G.J.B.). Publisher Copyright: © 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH

PY - 2021/1/26

Y1 - 2021/1/26

N2 - Glycans possess unparalleled structural complexity arising from chemically similar monosaccharide building blocks, configurations of anomeric linkages and different branching patterns, potentially giving rise to many isomers. This level of complexity is one of the main reasons that identification of exact glycan structures in biological samples still lags behind that of other biomolecules. Here, we introduce a methodology to identify isomeric N-glycans by determining gas phase conformer distributions (CDs) by measuring arrival time distributions (ATDs) using drift-tube ion mobility spectrometry-mass spectrometry . Key to the approach is the use of a range of well-defined synthetic glycans that made it possible to investigate conformer distributions in the gas phase of isomeric glycans in a systematic manner. In addition, we have computed CD fingerprints by molecular dynamics (MD) simulation, which compared well with experimentally determined CDs. It supports that ATDs resemble conformational populations in the gas phase and offer the prospect that such an approach can contribute to generating a library of CCS distributions (CCSDs) for structure identification.

AB - Glycans possess unparalleled structural complexity arising from chemically similar monosaccharide building blocks, configurations of anomeric linkages and different branching patterns, potentially giving rise to many isomers. This level of complexity is one of the main reasons that identification of exact glycan structures in biological samples still lags behind that of other biomolecules. Here, we introduce a methodology to identify isomeric N-glycans by determining gas phase conformer distributions (CDs) by measuring arrival time distributions (ATDs) using drift-tube ion mobility spectrometry-mass spectrometry . Key to the approach is the use of a range of well-defined synthetic glycans that made it possible to investigate conformer distributions in the gas phase of isomeric glycans in a systematic manner. In addition, we have computed CD fingerprints by molecular dynamics (MD) simulation, which compared well with experimentally determined CDs. It supports that ATDs resemble conformational populations in the gas phase and offer the prospect that such an approach can contribute to generating a library of CCS distributions (CCSDs) for structure identification.

KW - carbohydrates

KW - chemo-enzymatic synthesis

KW - conformations

KW - ion mobility spectrometry

KW - mass spectrometry

KW - molecular dynamics

UR - https://www.scopus.com/pages/publications/85099433832

U2 - 10.1002/chem.202004522

DO - 10.1002/chem.202004522

M3 - Article

C2 - 33047840

SN - 0947-6539

VL - 27

SP - 2149

EP - 2154

JO - Chemistry-A European Journal

JF - Chemistry-A European Journal

IS - 6

ER -