Biochemical Aspects of High-Resolution Mass Spectrometry

Ge, VanLear; Fw, McLafferty

doi:10.1146/annurev.bi.38.070169.001445

Cited by 29 publications

(11 citation statements)

References 68 publications

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“…A given species cannot be reasonably attributed to an experimental mass in either case due to the high number of overlapping isotopic distributions. This uncertainty frustrated a clear demonstration of how higher resolution enables attainment of higher mass accuracy . Here, the correlation with MS1 data from monomers, obtained either from denaturing electrospray or via ejected monomers, did allow us to assert the atom composition of subunits and the inference that the majority of the complexity observed was due to the incomplete desolvation of these complexes.…”

Section: Resultsmentioning

confidence: 97%

“…While CDMS has already been utilized to improve the resolving power of ion traps, , the massive disparity between ion traps and FT instruments in terms of resolving power suggests that the full potential of individual ion workflows is largely unrealized. Here, we report the realization of that potential with isotopic resolution for tetrameric pyruvate kinase (232 kDa) and tetrameric β-galactosidase (466 kDa), both of which were previously analyzed using ion trap CDMS. , This work contributes to the decades-long evolution of mass spectrometry and will help future researchers obtain greater clarity on desolvation and molecular composition for ions and biological complexes of ever higher mass.…”

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confidence: 94%

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Isotopic Resolution of Protein Complexes up to 466 kDa Using Individual Ion Mass Spectrometry

et al. 2020

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Native mass spectrometry involves transferring large biomolecular complexes into the gas phase, enabling the characterization of their composition and stoichiometry. However, the overlap in distributions created by residual solvation, ionic adducts, and post-translational modifications creates a high degree of complexity that typically goes unresolved at masses above ∼150 kDa. Therefore, native mass spectrometry would greatly benefit from higher resolution approaches for intact proteins and their complexes. By recording mass spectra of individual ions via charge detection mass spectrometry, we report isotopic resolution for pyruvate kinase (232 kDa) and β-galactosidase (466 kDa), extending the limits of isotopic resolution for high mass and high m/z by >2.5-fold and >1.6-fold, respectively.

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Section: Resultsmentioning

confidence: 97%

mentioning

confidence: 94%

Isotopic Resolution of Protein Complexes up to 466 kDa Using Individual Ion Mass Spectrometry

et al. 2020

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“…The three groups used a CEC 21–110 with direct introduction of the sample into the ion source. Nevertheless, the use of MS for the determination of amino acid sequences in peptides was, at that time, no more than a promising alternative restricted to pure oligopeptides of not more than 10 residues 25…”

Section: Events From 1965 Through 1974mentioning

confidence: 99%

From large analogical instruments to small digital black boxes: 40 years of progress in mass spectrometry and its role in proteomics. Part I 1965–1984

Gelpí

2008

J. Mass Spectrom.

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“…Mass spectrometry (MS) has become one of the most sensitive, accurate and informative analytical tools for a broad community. The use of MS has flourished in both industry and research, with applications ranging from the analysis of simple residual gas mixtures to complex organic materials, providing an imposing testimony to the value of this technique . The desire to mass spectrometrically analyze large numbers of samples at the point‐of‐use in the areas of biomedical, clinical, environmental research and public safety monitoring led to the development of ambient ionization techniques.…”

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confidence: 99%

An ambient detection system for visualization of charged particles generated with ionization methods at atmospheric pressure

Hommersom

Syed

Eijkel

et al. 2015

Rapid Comm Mass Spectrometry

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RationaleWith the current state of the art detection of ions only taking place under vacuum conditions active pixel detectors that operate under ambient conditions are of particular interest. These detectors are ideally suited to study and characterize the charge distributions generated by ambient ionization sources. MethodsThe direct imaging capabilities of the active pixel detector are used to investigate the spatial distributions of charged droplets generated by three ionization sources, named electrospray ionization (ESI), paper spray ionization (PSI) and surface acoustic wave nebulization (SAWN). The ionization spray (ESI/PSI) and ionization plume (SAWN) originating from each source is directly imaged. The effect of source parameters such as spray voltage for ESI and PSI, and the angle of the paper spray tip on the charge distributions is investigated. Two types of SAWN liquid interface, progressive wave (PW) and standing wave (SW) are studied. ResultsDirect charge detection under ambient conditions is demonstrated using an active pixel detector. Direct charge distributions are obtained of weak, homogeneous/focussed and dispersed spray plumes by applying low, intermediate and high spray potentials, respectively, for ESI. Spray plume footprints obtained for various angles of PSI shows the possibility to focus the ion beam as a function of the paper angle. Differences between two designs of the SAWN interface are determined. Droplet charge flux changes are illustrated in a way similar to a total ion chromatogram. ConclusionsThe use of this active pixel detector allows the rapid characterization and optimization of different ambient ionization sources without the actual use of a mass spectrometer. Valuable illustrations are obtained of changes in spatial distribution and number of charges detected for ESI, PSI and SAWN ion plumes.

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Biochemical Aspects of High-Resolution Mass Spectrometry

Cited by 29 publications

References 68 publications

Isotopic Resolution of Protein Complexes up to 466 kDa Using Individual Ion Mass Spectrometry

Isotopic Resolution of Protein Complexes up to 466 kDa Using Individual Ion Mass Spectrometry

From large analogical instruments to small digital black boxes: 40 years of progress in mass spectrometry and its role in proteomics. Part I 1965–1984

An ambient detection system for visualization of charged particles generated with ionization methods at atmospheric pressure

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