ESI, APCI, and MALDI a Comparison of the Central Analytical Figures of Merit: Sensitivity, Reproducibility, and Speed

Covey, Thomas R.; Schneider, Bradley B.; Javaheri, Hassan; LeBlanc, J. C. Yves; Ivosev, Gordana; Corr, Jay J.; Kovarik, Peter

doi:10.1002/9780470588901.ch13

Cited by 21 publications

(27 citation statements)

References 45 publications

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“…In addition, as a form of chemical ionization, MALDI did not eliminate the requirement for sample preparation, a critical bottleneck in the highthroughput workflow. 11,12 Sampling speeds faster than 1 Hz using acoustic dispensing of picoliter-volume sample drops have been reported. 13 This approach, referred to as acoustic mist ionization (AMI), uses acoustic energy parameters that create a mist of picolitervolume sample droplets that drift to the vacuum entrance of the mass spectrometry (MS) analyzer where it is inhaled through a heated ion pipe to evaporate the drops to dimensions required for field ion emission.…”

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confidence: 99%

Operational Modes and Speed Considerations of an Acoustic Droplet Dispenser for Mass Spectrometry

Liu¹,

Berkel²,

Cox³

et al. 2020

Anal. Chem.

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Acoustic ejection mass spectrometry is a recently developed concept in which low nanolitervolume sample droplets are acoustically dispensed from microtiter plate wells into a continuous fluid transfer open-port interface for subsequent ionization at atmospheric pressure. This manuscript focuses on the acoustic droplet dispensing component of a prototype system, in particular the well-to-well sampling speed, droplet volume calibration, precision, reproducibility, and various modes of operation this device enables. A new method to measure the volume of individually dispensed droplets is presented to both aid method validation and potentially assist in the tuning of acoustic dispense parameters for samples having a wide range of viscosities and surface tensions. Acoustic dispensing modes of operation discussed are high-speed, well-to-well dispensing of individual nanoliter-scale droplets from microtiter plates, including the first demonstration of 1536-well compatibility using this approach. Multiple nanoliter-volume droplets per sampling event to increase detection dynamic range is described, and a "continuous infusion" mode to provide a low sample consumption sustained steady-state signal for analyte detection optimization, improved ion statistics and signal-to-noise ratio (S/N), or time for in-depth tandem mass spectrometry of the components in a sample is presented. The concept of "bar coding" using combinations of dispensed droplet patterns to register well-plate position to specific mass spectral signals is introduced, as well as judicious well-plate sample layout to enable assay "multiplexing" as a means to maximize well-to-well sample analysis throughput, is also demonstrated.

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confidence: 99%

Operational Modes and Speed Considerations of an Acoustic Droplet Dispenser for Mass Spectrometry

Liu¹,

Berkel²,

Cox³

et al. 2020

Anal. Chem.

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“…The control inherent to laser based techniques, such as MALDI, provides sampling flexibility and precision, which is extremely advantageous for high throughput and selective sampling, as well as for mass spectrometry (MS) imaging. , Conventional MALDI produces primarily singly charged analyte ions and is in general less soft than ESI. − The matrices employed can introduce undesirable artifacts to MS spectra and adversely affect pre-analysis sample processing for certain scenarios. Innovative solutions utilizing continuous flow liquid MALDI matrix coupled directly to vacuum for laser ionization have been developed to combine analysis with solution separation methods such as liquid chromatography. , As well, numerous techniques have been developed to enhance analyte charging by combining the laser irradiation of matrix, tissue or aqueous solutions, with a secondary ionization device, with great success. − Atmospheric pressure (AP) MALDI systems have been utilized to ablate matrix material into the heated transfer capillary of the mass spectrometer where both highly charged peptide and protein ions were produced in the high temperature region. , The technique has been extended for the direct analysis of solution-analyte mixtures, producing highly charged species without the need for applied voltage, nebulizing gas, volatile solvents or laser irradiation termed “laserspray”, , not to be confused with “laser spray” developed by Hiraoka et al as described later.…”

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Soft Picosecond Infrared Laser Extraction of Highly Charged Proteins and Peptides from Bulk Liquid Water for Mass Spectrometry

Pieterse

Robertson

et al. 2018

Anal. Chem.

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We report the soft laser extraction and production of highly charged peptide and protein ions for mass spectrometry directly from bulk liquid water at atmospheric pressure and room temperature, using picosecond infrared laser ablation. Stable ion signal from singly charged small molecules, as well as highly charged biomolecular ions, from aqueous solutions at low laser pulse fluence (∼0.3 J cm) is demonstrated. Sampling via single picosecond laser pulses is shown to extract less than 27 pL of volume from the sample, producing highly charged peptide and protein ions for mass spectrometry detection. The ablation and ion generation is demonstrated to be soft in nature, producing natively folded proteins ions under sample conditions described for native mass spectrometry. The method provides laser-based sampling flexibility, precision and control with highly charged ion production directly from water at low and near neutral pH. This approach does not require an additional ionization device or high voltage applied directly to the sample.

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“… 13 , 14 It may affect the sensitivity, precision, and accuracy of the assay and, thus, both the quantitative and qualitative analysis. 15 − 18 Thus, besides proper sample preparation (and also its cleanup, 14 − 17 , 19 if necessary), it is also important to optimize the ionization (as well as fragmentation) parameters to reduce background signals, minimize the formation of adducts, and maximize the signal-to-noise ratio improving the sensitivity of the MS detector with regard to analytes. Moreover, tandem mass spectrometry (MS/MS) or high-resolution mass spectrometry (HRMS) also provides structural information, thereby enabling the identification of analytes.…”

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confidence: 99%

Mass Spectrometry for Investigation of Natural Dyes in Historical Textiles: Unveiling the Mystery behind Safflower-Dyed Fibers

Lech

Nawała

Popiel

2021

J. Am. Soc. Mass Spectrom.

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Safflower ( Carthamus tinctorius L.) petals, depending on the nature of a dyeing bath, dye fibers yellow or red. This is due to the presence of two kinds of components, water-soluble yellow colorants and alkali-soluble red compounds. In this study, safflower-yellow- and safflower-red-dyed silk, cotton, and wool fibers were investigated using high- or ultrahigh-performance liquid chromatography hyphenated with spectrophotometry and tandem mass spectrometry (HPLC–UV–vis–ESI-MS/MS) and high-resolution Orbitrap mass spectrometry (HPLC–HESI-HRMS) in order to identify the natural dye in historical textiles. This way, several quinochalcone C -glycosides were separated and characterized. Their low- and high-resolution MS/MS spectra expanded the database of natural colorants in cultural heritage objects. Moreover, the colorless ct-markers (with a hitherto unknown structure) present in all safflower-dyed fabrics, regardless of the color or preservation conditions, were revealed to be E / Z stereoisomers of N 1 ,N 5 ,N 10 -tri- p -coumaroylspermidine. Since most of the standards was not available, discussion on possible molecular structures was provided. As a consequence, the analytical investigation of the reference fibers dyed with safflower demonstrated that the dye composition varies, depending on the dyeing conditions and type of fiber. Moreover, it was proven that carthamin, although alkali soluble, can be successfully released with a mild extraction method, without its hydrolysis under these conditions. The results helped us to characterize threads sampled from 16th to 18thcentury textiles of European and Near Eastern origin. It has completed the picture of natural dyes used in the most valuable textiles availed in liturgical vestments from the collections of Krakow churches.

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ESI, APCI, and MALDI a Comparison of the Central Analytical Figures of Merit: Sensitivity, Reproducibility, and Speed

Cited by 21 publications

References 45 publications

Operational Modes and Speed Considerations of an Acoustic Droplet Dispenser for Mass Spectrometry

Operational Modes and Speed Considerations of an Acoustic Droplet Dispenser for Mass Spectrometry

Soft Picosecond Infrared Laser Extraction of Highly Charged Proteins and Peptides from Bulk Liquid Water for Mass Spectrometry

Mass Spectrometry for Investigation of Natural Dyes in Historical Textiles: Unveiling the Mystery behind Safflower-Dyed Fibers

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