Direct comparison of matrix-assisted laser desorption/ionisation and electrospray ionisation in the analysis of gangliosides by Fourier transform mass spectrometry

Penn, Sharron G.; Cancilla, Mark T.; Green, M. Kirk; Lebrilla, Carlito B.

doi:10.1255/ejms.4

Cited by 39 publications

(51 citation statements)

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“…Clearly Cs ϩ cations have somewhat stabilized the molecular ion. This is consistent with previous reports [30], but the presence of so many ion types generated from the starting homolog pair bodes ill for analysis of mixtures of unknown species with variable numbers of sialic acid residues.…”

Section: Resultssupporting

confidence: 93%

“…The utility of mass spectral analysis of gangliosides by MALDI-FTMS has been demonstrated, but its application has been hampered by extensive metastable fragmentation when standard MALDI sources are employed [27,28,30,40,41], and derivatization, e.g., permethylation, is often necessary to stabilize the more highly labile species sufficiently to enable MS analysis. In the case of homogeneous standards, metastable fragmentation can be used to verify the details of the ganglioside structures, but for heterogenous samples like those typically extracted from biological tissues, extensive fragmentation during the analysis makes determination of the composition of the ganglioside mixtures extremely difficult or impossible.…”

Section: Resultsmentioning

confidence: 99%

“…With both Electrospray and MALDI mass spectrometry, the loss of sialic acid residues is the predominant fragmentation pathway. This property is particularly important for MALDI-FTMS where the relatively long time between ionization and detection (0.3-30 s depending on the resolution desired and the pumping efficiency of the specific vacuum system) allows unimolecular metastable fragmentation reactions to go to completion [28,30,32]. However, some methods have been developed to partially stabilize the gangliosides on desorption.…”

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confidence: 99%

“…In particular, cool matrices like 6-azo-2-thiothymine (ATT) [16] and 2-5-dihydroxybenzoic acid [33], having the property of decreasing the observed metastable decay in reflectron mode, were introduced in MALDI time of flight (TOF). Similarly, use of larger alkali cations [30], such as cesium, has been successful in reducing (but not eliminating) fragmentation of the gangliosides. Conversion of the carboxyl group to a methyl ester improves stability [18], as does permethylation [16], but derivatization is not an option when a bioassay is part of the overall characterization scheme.…”

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confidence: 99%

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High pressure matrix-assisted laser desorption/ionization Fourier transform mass spectrometry for minimization of ganglioside fragmentation

O’Connor

Mirgorodskaya

Costello

2002

J. Am. Soc. Mass Spectrom.

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Transiently elevating pressure in a matrix-assisted laser desorption/ionization Fourier transform mass spectrometry (MALDI-FTMS) source into the 1-10 mbar range during ionization decreases the metastable fragmentation of gangliosides. This allows detection of the molecular ion species without loss of the highly labile sialic acid residues. In these experiments, gangliosides with up to five sialic acids were ionized by MALDI and detected with the FTMS. In each case, when the high pressure collisional cooling was used, the singly charged molecular ion was the base peak in the spectra, both in the positive and negative ion modes, and minimal metastable fragmentation was observed. This result is promising, as the previously developed TLC separation methods can be coupled to MALDI-FTMS. (J Am Soc Mass Spectrom 2002, 13, 402-407)

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Section: Resultssupporting

confidence: 93%

Section: Resultsmentioning

confidence: 99%

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confidence: 99%

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High pressure matrix-assisted laser desorption/ionization Fourier transform mass spectrometry for minimization of ganglioside fragmentation

O’Connor

Mirgorodskaya

Costello

2002

J. Am. Soc. Mass Spectrom.

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“…An interesting comparison of the MALDI-TOF and ESI FT-ICR MS techniques for the analysis of gangliosides has been provided by Penn et al (1997). The ESI and the MALDI spectra were both obtained.…”

Section: Oligosaccharides and Glycoconjugatesmentioning

confidence: 99%

Development of new methodologies for the mass spectrometry study of bioorganic macromolecules

Cristoni

Bernardi

2003

Mass Spectrometry Reviews

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I. Introduction 370 II. Techniques That Are Usually Employed in the Study of Bioorganic Macromolecules 371 A. Proteins and Peptides 371 B. Oligonucleotides 374 C. Oligosaccharides and Glycoconjugates 375 D. Various Complexes (DNA–Protein, Antigen–Antibody, Macromolecules–Metals) 377 III. Common Problems and Developments in the Analysis of Bioorganic Macromolecules by Mass Spectrometry 377 A. Ionization Source Problems and Developments 377 1. Sensitivity 377 2. Problems with Buffers 379 3. Multicharge Effect 381 B. Mass Analyzer Problems and Developments 381 1. Linear Dynamic Range 381 2. Tandem Mass Spectrometry 382 3. Sensitivity 382 4. Resolution 383 5. Mass Accuracy 383 IV. New Promising Technologies 384 A. Interfaces and Ionization Sources 384 1. Improvements in the Coupling of Liquid‐Phase Separation Systems to Mass Spectrometry 384 2. AP‐MALDI 384 3. Deprotonant Agents 385 4. Sonic Spray Ionization 388 5. APCI without Corona Discharge 391 B. Mass Analyzers 393 1. Linear Quadrupole Ion Trap 394 2. TOF Analyzers with New Detectors 395 3. Multiple Mass Analyzers 396 V. Software for Data Treatment 397 VI. Conclusions and Future Developments 399 Acknowledgments 400 References 400 In recent years, mass spectrometry has been increasingly used for the analysis of various macromolecules of biological, biomedical, and biochemical interest. This increase has been made possible by two key developments: the advent of electrospray ionization (ESI) and matrix‐assisted laser desorption ionization (MALDI) sources. The two new techniques produce a significant increase in mass range and in sensitivity that led to the development of new applications and of new analyzer designs, software, and robotics. This review, apart from the description of the status of mass spectrometry in the analysis of bioorganic macromolecules, is mainly devoted to the illustration of the more recent promising techniques and on their possible future evolution. © 2003 Wiley Periodicals, Inc., Mass Spec Rev 22:369–406, 2003; Published online in Wiley InterScience (www.interscience.wiley.com). DOI 10.1002/mas.10062

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Direct matrix-assisted laser desorption/ionization mass spectrometric analysis of glycosphingolipids on thin layer chromatographic plates and transfer membranes

Guittard

Hronowski

Costello

1999

Rapid Commun. Mass Spectrom.

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Results are reported for analysis by matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOFMS) of native glycosphingolipids (GSLs) after development on thin layer chromatographic plates and after heat transfer of the GSLs from the plates to several types of polymer membranes. The spectral quality is better for membrane-bound analytes, in terms of sensitivity, mass resolution and background interference. The sensitivity gain compared with liquid secondary ion mass spectrometry (LSIMS) of GSLs on thin layer plates is 1-2 orders of magnitude (detection limits of 5-50 pmol vs. 1-10 nmol). Resolution and mass accuracy (0.1%) are limited by the irregular membrane surfaces and this effect cannot be entirely compensated by delayed extraction. The best results were obtained with a polyvinylidene difluoride (PVDF) P membrane, with irradiation from a nitrogen laser. Although the Nafion membrane could not be used for molecular weight profiling, its acidic character led to sample hydrolysis at the glycosidic linkages, thus yielding a series of fragments that could be used to determine the sequence of carbohydrate residues. Structural information could also be obtained by post-source decay (PSD) experiments on mass-selected precursor ions. Samples containing both neutral and acidic components were characterized in a 1:1 combination of 2, 5-dihydroxybenzoic acid and 2-amino-5-nitropyridine. GSLs that exhibited binding to antibodies in an overlay assay on the TLC plate were transferred to membranes and analyzed by MALDI-TOFMS without interference from the antibody or the salts and buffers used during the binding and visualization steps. Taking advantage of the insights into sample preparation gained from these studies, future research will extend this approach to analysis by matrix-assisted laser desorption/ionization Fourier transform ion cyclotron resonance mass spectrometry (MALDI-FTICRMS) with an external ion source.

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Direct comparison of matrix-assisted laser desorption/ionisation and electrospray ionisation in the analysis of gangliosides by Fourier transform mass spectrometry

Cited by 39 publications

References 2 publications

High pressure matrix-assisted laser desorption/ionization Fourier transform mass spectrometry for minimization of ganglioside fragmentation

High pressure matrix-assisted laser desorption/ionization Fourier transform mass spectrometry for minimization of ganglioside fragmentation

Development of new methodologies for the mass spectrometry study of bioorganic macromolecules

Direct matrix-assisted laser desorption/ionization mass spectrometric analysis of glycosphingolipids on thin layer chromatographic plates and transfer membranes

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