High‐field‐magnet mass spectrometry of biological molecules

Dell, Anne; Taylor, Graham W.

doi:10.1002/mas.1280030303

Cited by 41 publications

(7 citation statements)

References 79 publications

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“…During the last three decades, a vast number of MS-based methods have been developed that were specifically tailored to obtain insight into the different aspects of glycoconjugate structures including GSLs. Among these, fast atom bombardment (FAB), secondary ion (SI), electron ionization (EI), and matrix-assisted laser desorption/ionization (MALDI) MS have been found to be especially powerful for determining (a) molecular masses of oligosaccharides up to the range of more than 30 sugar units, (b) sequence and pattern branching, and (c) structure of the aglycon (Reinhold & Carr, 1983;Dell & Taylor, 1984;Egge & Peter-Katalinić, 1987;Peter-Katalinić, 1994;Miller-Podraza, 2000). However, it has to be stressed that a complete structural elucidation always has to resort to additional methods like high-resolution nuclear magnetic resonance spectroscopy (Sweeley & Nunez, 1985;Yu et al, 1986;Dabrowski, 1989), chemical or enzymic degradation, and gas chromatography (GC) MS analysis of partially methylated alditol acetates derived from permethylated compounds (''methylation analysis'') (Levery & Hakomori, 1987;Hanisch, 1994;Geyer & Geyer, 1998), just to mention a few.…”

Section: Mass Spectrometrymentioning

confidence: 99%

Advances on the compositional analysis of glycosphingolipids combining thin-layer chromatography with mass spectrometry

Müthing

Distler

2009

Mass Spectrom. Rev.

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Glycosphingolipids (GSLs), composed of a hydrophilic carbohydrate chain and a lipophilic ceramide anchor, play pivotal roles in countless biological processes, including infectious diseases and the development of cancer. Knowledge of the number and sequence of monosaccharides and their anomeric configuration and linkage type, which make up the principal items of the glyco code of biologically active carbohydrate chains, is essential for exploring the function of GSLs. As part of the investigation of the vertebrate glycome, GSL analysis is undergoing rapid expansion owing to the application of novel biochemical and biophysical technologies. Mass spectrometry (MS) takes part in the network of collaborations to further unravel structural and functional aspects within the fascinating world of GSLs with the ultimate aim to better define their role in human health and disease. However, a single-method analytical MS technique without supporting tools is limited yielding only partial structural information. Because of its superior resolving power, robustness, and easy handling, high-performance thin-layer chromatography (TLC) is widely used as an invaluable tool in GSL analysis. The intention of this review is to give an insight into current advances obtained by coupling supplementary techniques such as TLC and mass spectrometry. A retrospective view of the development of this concept and the recent improvements by merging (1) TLC separation of GSLs, (2) their detection with oligosaccharide-specific proteins, and (3) in situ MS analysis of protein-detected GSLs directly on the TLC plate, are provided. The procedure works on a nanogram scale and was successfully applied to the identification of cancer-associated GSLs in several types of human tumors. The combination of these two supplementary techniques opens new doors by delivering specific structural information of trace quantities of GSLs with only limited investment in sample preparation.

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Section: Mass Spectrometrymentioning

confidence: 99%

Advances on the compositional analysis of glycosphingolipids combining thin-layer chromatography with mass spectrometry

Müthing

Distler

2009

Mass Spectrom. Rev.

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“…Anomers and linkage isomers that have identical masses cannot be easily distinguished in mass spectrometry, but to aid in this endeavor, separation steps are often performed before mass spectrometric identification. Nevertheless, MS does have the capability to differentiate underivatized saccharide stereoisomers as demonstrated when coupled with several different desorption/ionization techniques such as field desorption (FD) [3,4], laser desorption (LD) [5,6], fast atom bombardment (FAB) [7][8][9][10][11][12][13][14][15][16][17], liquid secondary ion mass spectrometry (LSIMS) [18,19], and electrospray (ES) [20 -25].…”

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confidence: 99%

MALDI linear-field reflectron TOF post-source decay analysis of underivatized oligosaccharides: Determination of glycosidic linkages and anomeric configurations using anion attachment

Guan

Cole

2008

J. Am. Soc. Mass Spectrom.

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Six different anionic species (fluoride, chloride, bromide, iodide, nitrate, and acetate) are tested for their abilities to form anionic adducts with neutral oligosaccharides that are detectable by MALDI-TOF mass spectrometry. Fluoride and acetate cannot form anionic adducts with the oligosaccharides in significant yields. However, bromide, iodide, and nitrate anionic adducts consistently appear in higher abundances relative to [M Ϫ H] Ϫ , just like the highly stable chloride adducts. Post-source decay (PSD) decompositions of Br Ϫ , IϪ , and NO 3 Ϫ adducts of oligosaccharides provide no structural information, i.e., they yield the respective anions as the main product ions. However, determination of linkage types is achieved by analysis of structurally-informative diagnostic peaks offered by negative ion PSD spectra of chloride adducts of oligosaccharides, whereas the relative peak intensities of pairs of diagnostic fragment ions allow differentiation of anomeric configurations of glycosidic bonds. Thus, simultaneous identification of the linkage types and anomeric configurations of glycosidic bonds is achieved. Our data indicate that negative ion PSD fragmentation patterns of chloride adducts of oligosaccharides are mainly determined by the linkage types. Correlation may exist between the linkage positions and fragmentation mechanisms and/or steric requirements for both cross-ring and glycosidic bond fragmentations. PSD of the chloride adducts of saccharides containing a terminal Glc␣1-2Fru linkage also yields chlorine-containing fragment ions which appear to be specifically diagnostic for a fructose linked at the 2-position on the reducing end. This also allows differentiation from saccharides with a 1-1 linked pyranose on the same position. ollowing the advances in proteomics, there is a growing interest in the importance of glycomics, i.e., the study of the breadth of sugar forms (structure and function of glycans) in biological organisms. Carbohydrates (or saccharides) are the most abundant biological compounds found on earth. They are well known as energy reservoirs and structural materials in cell walls. However, it has become clear that oligosaccharides and glycoconjugates (e.g., glycoproteins and glycolipids) serve as crucial mediators for a wide variety of complex cellular events [1]. Carbohydrates also play an important role in specific molecular recognition, protein folding, stability, and pharmacokinetics due to their great structural diversity. Moreover, glycosylation is a ubiquitous form of post-translational modification to both proteins and lipids.Gaining a clear understanding of the crucial biological roles of oligosaccharides requires complete structural characterization of carbohydrates or glycoconjugates, which includes determinations of the numbers and types of monosaccharide units, ring substituents, sequences, branching, linkage positions, and anomeric configurations between adjacent monosaccharide units. In most cases, merely knowing the monosaccharide sequence is inadequate; thus, unam...

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“…Other methods implementing the derivatization of saccharides have been used to obtain their structural information [3][4][5][6][7][8][9][10][11]. The soft mass spectrometry ionization techniques such as fast atom bombardment (FAB) [12][13][14][15][16], liquid secondary ionization mass spectrometry (LSIMS) [17,18], along with matrix-assisted laser desorption ionization (MALDI) [19 -23], and electrospray ionization (ESI) [24 -28] have gained attention as approaches to investigate underivatized oligosaccharides. Collision-induced dissociation (CID) offers the possibility to assign details of carbohydrate structure such as sugar sequence for linear oligosaccharides [12], linkage position [12,[15][16][17]29], and differentiation of anomers [25,30].…”

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confidence: 99%

Rapid and sensitive differentiation of anomers, linkage, and position isomers of disaccharides using High-Field Asymmetric Waveform Ion Mobility Spectrometry (FAIMS)

Gabryelski

Froese

2003

J. Am. Soc. Mass Spectrom.

127

124

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A challenging aspect of structural elucidation of carbohydrates is gaining unambiguous information for anomers, linkage, and position isomers. Such isomers with identical mass can't be easily distinguished in mass spectrometry and a separation step is required prior to mass spectrometry identification. In our laboratory, gas-phase separation and differentiation of anomers, linkage, and position isomers of disaccharides was achieved using High-Field Asymmetric Waveform Ion Mobility Spectrometry (FAIMS). The FAIMS method responds to changes in ion mobility at high field rather than absolute values of ion mobility, and was shown to provide efficient separation and identification of disaccharide isomers at high sensitivity. Separation of analyzed disaccharide isomers can be accomplished at low nM level in a matter of seconds without sample purification or fractionation. Capability for examining a large population of ionic species of disaccharides by this method allowed for correlating structural details of disaccharide isomers with their separation properties in FAIMS. Results for disaccharide isomers indicate that this method could be applied to a larger group of carbohydrates. ( Mass spectrometry has shown a unique ability to resolve certain structural ambiguities. Permethylation is a well developed but time-consuming GC-MS method in linkage analysis of oligosaccharides [1,2]. Other methods implementing the derivatization of saccharides have been used to obtain their structural information [3][4][5][6][7][8][9][10][11]. The soft mass spectrometry ionization techniques such as fast atom bombardment (FAB) [12][13][14][15][16], liquid secondary ionization mass spectrometry (LSIMS) [17,18], along with matrix-assisted laser desorption ionization (MALDI) [19 -23], and electrospray ionization (ESI) [24 -28] have gained attention as approaches to investigate underivatized oligosaccharides. Collision-induced dissociation (CID) offers the possibility to assign details of carbohydrate structure such as sugar sequence for linear oligosaccharides [12], linkage position [12,[15][16][17]29], and differentiation of anomers [25,30]. In addition to analyzing protonated or deprotonated molecular ions of saccharides in CID, alkali metal adduct ions have been used to promote fragmentation of ligand-carbohydrate complexes. In the positive ion mode, calcium and magnesium adducts of oligosaccharides were investigated for the elucidation of the linkage position of trisaccharides [26] and cobalt complexes have been used to differentiate the anomeric configuration of disaccharides [30]. In the negative ion mode, decomposition of chloride adducts was investigated for differentiation of the linkage position of disaccharides [31].Despite recent advances in tandem mass spectrometry of carbohydrates, the spectral differences for some isomers are very small and they do not provide unambiguous identification. This is especially true when a mixture of isomers with the same m/z has to be analyzed. In such applications a separation step is required ...

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High‐field‐magnet mass spectrometry of biological molecules

Cited by 41 publications

References 79 publications

Advances on the compositional analysis of glycosphingolipids combining thin-layer chromatography with mass spectrometry

Advances on the compositional analysis of glycosphingolipids combining thin-layer chromatography with mass spectrometry

MALDI linear-field reflectron TOF post-source decay analysis of underivatized oligosaccharides: Determination of glycosidic linkages and anomeric configurations using anion attachment

Rapid and sensitive differentiation of anomers, linkage, and position isomers of disaccharides using High-Field Asymmetric Waveform Ion Mobility Spectrometry (FAIMS)

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