Lipid/Peptide/Nucleotide Separation with MALDI-Ion Mobility-TOF MS

Woods, Amina S.; Ugarov, M. V.; Egan, Thomas F.; Koomen, John M.; Gillig, Kent J.; Führer, Katrin; Gonin, Marc; Schultz, J.

doi:10.1021/ac035376k

Cited by 147 publications

(137 citation statements)

References 22 publications

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“…This parameter determines the "tightness" of a given gap width, and thus is critical in the design of FAIMS separations 47 and also HODIMS, as discussed below. As a corollary of eq (1): (17) where C E is a numerical coefficient (0 < C E < 1) that depends on the waveform profile. For eqs (14/14′), C E ≅ 0.3236, which is slightly lower than C E = 1/3 in FAIMS.…”

Section: Fundamental Feasibility Of Higher-order Differential Ion Mobmentioning

confidence: 99%

“…Other factors being equal, the gap would ideally be somewhat wider than for FAIMS, with the waveform voltage scaled to establish the same E D . Alternatively, one could increase w in proportion to C E E D /N to produce constant Δ r by eq (17). Regardless, these estimates suggest that HODIMS could use existing FAIMS mechanical hardware, allowing a rapid switching between all n ≥ 2 orders on the software level by changing only the E(t) profile and possibly adjusting the amplitude and/or frequency.…”

Section: Gap Width and Waveform Frequencymentioning

confidence: 99%

“…[4][5][6][7][8][9][10] Recent commercial introduction of such systems [11][12][13][14] is expanding interest in ion mobility/MS, particularly for analyses of complex biological samples such as proteolytic digests and lipids, nucleotides, and metabolites. [15][16][17][18][19][20][21][22][23][24] Single-stage ion mobility spectrometry (IMS) was investigated since the 1970s, [25][26][27] with a noteworthy development of ESI/IMS in 1980s. 28 In IMS, ions drift through a non-reactive buffer gas under the influence of a modest electric field.…”

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Feasibility of Higher-Order Differential Ion Mobility Separations Using New Asymmetric Waveforms

2006

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Technologies for separating and characterizing ions based on their transport properties in gases have been around for three decades. The early method of ion mobility spectrometry (IMS) distinguished ions by absolute mobility that depends on the collision cross section with buffer gas atoms. The more recent technique of field asymmetric waveform IMS (FAIMS) measures the difference between mobilities at high and low electric fields. Coupling IMS and FAIMS to soft ionization sources and mass spectrometry (MS) has greatly expanded their utility, enabling new applications in biomedical and nanomaterials research. Here, we show that time-dependent electric fields comprising more than two intensity levels could, in principle, effect an infinite number of distinct differential separations based on the higher-order terms of expression for ion mobility. These analyses could employ the hardware and operational procedures similar to those utilized in FAIMS. Methods up to the 4 th or 5 th order (where conventional IMS is 1 st order and FAIMS is 2 nd order) should be practical at field intensities accessible in ambient air, with still higher orders potentially achievable in insulating gases. Available experimental data suggest that higher-order separations should be largely orthogonal to each other and to FAIMS, IMS, and MS.Approaches to separation of ion mixtures and characterization of ions in the gas phase based on ion mobility are becoming commonplace in analytical chemistry. The key advantage of gas-phase separations over condensed phase methods is the exceptional speed enabled by rapid molecular motion in gases. This inherent benefit is made increasingly topical by the growing focus of analytical technology on higher throughput. Since their first demonstration a decade ago, 1-3 instrumental platforms combining electrospray ionization (ESI) or matrixassisted laser desorption ionization (MALDI) sources with ion mobility separations and mass-spectrometry (MS) have undergone a sustained development that has improved their resolution and sensitivity to the levels demanded by practical applications. 4-10 Recent commercial introduction of such systems 11-14 is expanding interest in ion mobility/MS, particularly for analyses of complex biological samples such as proteolytic digests and lipids, nucleotides, and metabolites. [15][16][17][18][19][20][21][22][23][24] Single-stage ion mobility spectrometry (IMS) was investigated since the 1970s, 25-27 with a noteworthy development of ESI/IMS in 1980s. 28 In IMS, ions drift through a non-reactive buffer gas under the influence of a modest electric field. The drift velocity (v) in the field of intensity E is determined by ion mobility (K):(1)For consistency, measured mobilities are normally converted to reduced values K 0 by adjusting the buffer gas temperature (T, Kelvin) and pressure (P, Torr) to standard (STP) conditions:NIH Public Access

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Section: Fundamental Feasibility Of Higher-order Differential Ion Mobmentioning

confidence: 99%

Section: Gap Width and Waveform Frequencymentioning

confidence: 99%

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confidence: 99%

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Feasibility of Higher-Order Differential Ion Mobility Separations Using New Asymmetric Waveforms

2006

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“…Growth was scraped from the agar plates and washed twice with 200 mL sterile water, resuspended in sterile water, heat-killed, and lyophilized. The vegetative cells were prepared by suspending isolated colonies from TSA and sheep's blood agar plates in sterile water to a density corresponding to a 1-McFarland standard.2 9 This was diluted 1:10, and 2 mL of the 1:10 suspension was added to 200 mL of nutrient broth. The nutrient broth was incubated overnight at ambient temperature, centrifuged, and washed twice with 200-mL sterile water.…”

Section: 2mentioning

confidence: 99%

Correlation of Mass Spectrometry Identified Bacterial Biomarkers from a Fielded Pyrolysis-Gas Chromatography-Ion Mobility Spectrometry Biodetector with the Microbiological Gram Stain Classification Scheme

et al. 2004

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Public reporting burden for fthi collection of Informaiaon is estimated to, average I hour per response, including the time for reviewing Instructions. searchilng erristing data sources, gatheing and maintsteng the data needed, and completing and review"n this collection of Information. Send cofmment regarding this burden estimate or any othier aspect of this collection of Infomuation, Indluding suggestions for reducing fti burden to Departmrent PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) AND ADDRESS(ES) 8. PERFORMING ORGANIZATION REPORTDIR ECBC, ATTN: AMSRD-ECBC-RT-II, APG, MD 21010-5424 NUMBER GEO-CENTERS, Inc., Gunpowder Branch, APG, MD 21010-5424 ECBC-TR-415 SPONSORING / MONITORING AGENCY NAME(S) AND ADDRESS(ES) 10. SPONSORIMONITOR'S ACRONYM(S) SPONSORIMONITOR'S REPORT NUMBER(S) DISTRIBUTION I AVAILABILITY STATEMENTApproved for public release; distribution is unlimited. SUPPLEMENTARY NOTES ABSTRACTThis work discusses the significance of the pyrolyzate peaks observed in the gas chromatography-ion mobility spectrometry (GC-IMS) dataspace of the pyrolysis-GC-IMS (Py-GC-IMS) briefcase system. This system has the ability to detect and classifyi deliberately released bioaerosols in outdoor field scenarios. The bioaerosols include Gram-positive spores and Gram-negative bacteria, the MS-2 Escherichia coliphage virus, and ovalbumnin (OV) protein species. The work suggests certain improvements that can be made to the IMS detection System. A pyrolysis-gas chromatography-ion mobility spectrometry (Py-GC-IMS) briefcase system can detect and classify deliberately released bioaerosols in outdoor field scenarios. The bioaerosols include Gram-positive spores and Gram-negative bacteria, the MS-2 Escherichia coliphage virus, and ovalbumin (OV) protein species. However, the origin and structural identities of the pyrolyzate peaks observed in the GC-IMS dataspace, their microbiological information content, and taxonomic importance with respect to biodetection have not been determined. SUBJECT TERMS PyrolysisThe present work interrogates the identities of the peaks by inserting a time-offlight (TOF) mass spectrometry (MS) system in parallel with the IMS detector through a Tee connection in the GC module. Biological substances, producing ion mobility peaks from the pyrolysis of microorganisms, have been identified by their GC retention times, by matching their electron ionization mass spectra with authentic standards, and by the National Institute of Standards and Technology (NIST) mass spectral database.Strong signals from 2-pyridinecarboxamide were identified in Bacillus samples, including Bacillus anthracis, and their origins were traced to the cell wall peptidoglycan macromolecule. 3-Hydroxymyristic acid is a component of lipopolysaccharides (LPS) in the cell walls of Gram-negative organisms. The Gram-negative E. coli organism showed significant amounts of 3-Hydroxymyristic acid derivatives and degradation products in Py-GC-MS analyses. Some of the fatty acid derivatives were observed in very low abundance in the ion mobi...

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“…Peptides, for instance, generally have more compact structures compared with lipids of the same mass range. Thus, an m/z versus mobility diagram of a mixture of peptides and lipids upon IMS-MS analysis shows two distinct patterns [10,11].…”

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confidence: 99%

Applying a dynamic method to the measurement of ion mobility

Baykut

Halem

Raether

2009

J. Am. Soc. Mass Spectrom.

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A dynamic method is applied to measure the mobility of gas-phase ions in the dual ion funnel interface of the electrospray source of a quadrupole orthogonal time-of-flight mass spectrometer. In a new operational mode, a potential barrier was formed in the second ion funnel of the mass spectrometer and then progressively increased. In this region, a flow of gas drags the ions into the mass spectrometer while the electric force applied by the potential barrier decelerates them. Ions with lower mobility can be carried by the gas flow more easily than those with high mobility. Thus, electrical forces can block the more mobile ions more easily. Hence, the electric barrier formed in the ion funnel permits only ions below a certain mobility threshold to enter the mass spectrometer. When the barrier voltage is increased, this threshold moves from high to low mobilities. Ions with mobilities above the threshold cannot enter the mass spectrometer, and their signal decreases to zero. Thus, in a barrier voltage scan, mass spectrometric signals of ions sequentially disappear. Differentiation of these decreasing ion signal curves produces peaks from which an ion mobility spectrum can be reconstructed. Blocking voltages, i.e., the positions of the peaks on the barrier voltage scale are directly related to the mobility of these ions. An internal calibration using ions with known mobility values helps determine the unknown ion mobilities and allows calculation of ionic cross sections. (J Am Soc Mass

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Lipid/Peptide/Nucleotide Separation with MALDI-Ion Mobility-TOF MS

Cited by 147 publications

References 22 publications

Feasibility of Higher-Order Differential Ion Mobility Separations Using New Asymmetric Waveforms

Feasibility of Higher-Order Differential Ion Mobility Separations Using New Asymmetric Waveforms

Correlation of Mass Spectrometry Identified Bacterial Biomarkers from a Fielded Pyrolysis-Gas Chromatography-Ion Mobility Spectrometry Biodetector with the Microbiological Gram Stain Classification Scheme

Applying a dynamic method to the measurement of ion mobility

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