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Article ; Online: The triple quadrupole: Innovation, serendipity and persistence.

Yost, Richard A

Journal of mass spectrometry and advances in the clinical lab

2022 Volume 24, Page(s) 90–99

Language	English
Publishing date	2022-05-10
Publishing country	Netherlands
Document type	Journal Article
ISSN	2667-145X
ISSN (online)	2667-145X
DOI	10.1016/j.jmsacl.2022.05.001
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Article ; Online: Why tandem mass spectrometry for trace analysis: Concepts of tandem analytical techniques.

Yost, Richard A

Rapid communications in mass spectrometry : RCM

2022 Volume 36, Issue 13, Page(s) e9310

Abstract: Rationale: The triple quadrupole mass spectrometer, typically in combination with a gas or liquid chromatograph (GC/MS/MS and LC/MS/MS), is perhaps the most iconic example today of a tandem analytical instrument. Here I present the concepts of tandem or ...

Abstract	Rationale: The triple quadrupole mass spectrometer, typically in combination with a gas or liquid chromatograph (GC/MS/MS and LC/MS/MS), is perhaps the most iconic example today of a tandem analytical instrument. Here I present the concepts of tandem or hyphenated techniques for trace analysis (that is, the detection and/or quantitation of one or more analytes present in a mixture at low levels). Methods: This tutorial presents the principles of tandem trace analytical techniques such as GC/MS/MS and LC/MS/MS, including the capabilities and requirements for such tandem techniques, the role of sensitivity and selectivity in tandem techniques, ways to assess the "informing power" of these techniques, and a comparison of tandem techniques with individual techniques at high resolution. These points are illustrated with several examples of trace analysis using tandem analytical techniques. Results: Several characteristics of the triple quadrupole have made it the "laboratory workhorse" for trace analysis, including the remarkable efficiency of the low-energy collision-induced dissociation (CID) process in a radiofrequency (RF)-only multipole collision cell, the ease of computer control, and the capability for rapid scanning, rapid switching from mass to mass, and high transmission efficiency, enabling a wide variety of MS/MS scans. The efficiency of selected reaction monitoring means that triple quadrupoles dominate MS/MS for detection and quantitation of targeted compounds. Conclusions: This special issue addresses the intriguing question of how the triple quadrupole mass spectrometer progressed from "bleeding edge" to "the laboratory workhorse" over the last 40 years. This tutorial on the principles of tandem trace analytical techniques provides perspectives and insights into answering that question and should help educate the novice and stimulate the sophisticate.
MeSH term(s)	Chromatography, Liquid/methods ; Tandem Mass Spectrometry/methods
Language	English
Publishing date	2022-05-02
Publishing country	England
Document type	Journal Article
ZDB-ID	58731-x
ISSN	1097-0231 ; 0951-4198
ISSN (online)	1097-0231
ISSN	0951-4198
DOI	10.1002/rcm.9310
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Article ; Online: Characterization of Bile Acid Isomers and the Implementation of High-Resolution Demultiplexing with Ion Mobility-Mass Spectrometry.

Kemperman, Robin H J / Chouinard, Christopher D / Yost, Richard A

Journal of the American Society for Mass Spectrometry

2023 Volume 34, Issue 7, Page(s) 1477–1490

Abstract: Bile acids (BAs) are a complex suite of clinically relevant metabolites that include many isomers. Liquid chromatography coupled to mass spectrometry (LC-MS) is an increasingly popular technique due to its high specificity and sensitivity; nonetheless, ... ...

Abstract	Bile acids (BAs) are a complex suite of clinically relevant metabolites that include many isomers. Liquid chromatography coupled to mass spectrometry (LC-MS) is an increasingly popular technique due to its high specificity and sensitivity; nonetheless, acquisition times are generally 10-20 min, and isomers are not always resolved. In this study, the application of ion mobility (IM) spectrometry coupled to MS was investigated to separate, characterize, and measure BAs. A subset of 16 BAs was studied, including three groups of isomers belonging to unconjugated, glycine-conjugated, and taurine-conjugated BA classes. A variety of strategies were explored to increase BA isomer separation such as changing the drift gas, measuring different ionic species (i.e., multimers and cationized species), and enhancing the instrumental resolving power. In general, Ar, N
Language	English
Publishing date	2023-06-15
Publishing country	United States
Document type	Journal Article
ZDB-ID	1073671-2
ISSN	1879-1123 ; 1044-0305
ISSN (online)	1879-1123
ISSN	1044-0305
DOI	10.1021/jasms.3c00143
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Article ; Online: Segmented Flow Strategies for Integrating Liquid Chromatography–Mass Spectrometry with Nuclear Magnetic Resonance for Lipidomics

Lei, Jiajun / Mahar, Rohit / Chang, Mario C. / Collins, James / Merritt, Matthew E. / Garrett, Timothy J. / Yost, Richard A.

Analytical Chemistry. 2023 Jan. 11, v. 95, no. 3 p.1908-1915

2023

Abstract: Building an accurate lipid inventory relies on coordinated information from orthogonal analytical capabilities. Integrating the familiar workflow of liquid chromatography (LC), high-resolution mass spectrometry (HRMS), and tandem mass spectrometry (MS/MS) ...

Abstract	Building an accurate lipid inventory relies on coordinated information from orthogonal analytical capabilities. Integrating the familiar workflow of liquid chromatography (LC), high-resolution mass spectrometry (HRMS), and tandem mass spectrometry (MS/MS) with proton nuclear magnetic resonance spectroscopy (¹H NMR) would be ideal for building that inventory. For absolute lipid structural elucidation, LC–HRMS/MS can provide lower-level structural information with superior sensitivity, while ¹H NMR can provide invaluable higher-order structural information for the disambiguation of isomers with absolute chemical specificity. Digitization of the LC eluent followed by splitting the microfractions into two flow paths in a defined ratio for HRMS/MS and NMR would be the ideal strategy to permit correlation of the MS and NMR data as a function of chromatographic retention time. Here, we report an active segmentation platform to transform analytical flow rate LC eluent into parallel microliter segmented flow queues for high confidence correlation of the MS, MS/MS, and NMR data. The practical details in implementing this strategy to achieve an integrated LC–MS–NMR platform are presented, including the development of an active segmentation technology using a four-port two-way valve to transform the LC eluent into parallel segmented flows for online MS analysis followed by offline segment-specific ¹H NMR and optimization of the detector response toward segmented flow. To demonstrate the practicality of this novel platform, it was tested using lipid mixture samples.
Keywords	analytical chemistry ; inventories ; lipidomics ; lipids ; liquid chromatography ; nuclear magnetic resonance spectroscopy ; tandem mass spectrometry
Language	English
Dates of publication	2023-0111
Size	p. 1908-1915.
Publishing place	American Chemical Society
Document type	Article ; Online
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.2c03974
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Article: A rapid and robust method for amino acid quantification using a simple N-hydroxysuccinimide ester derivatization and liquid chromatography-ion mobility-mass spectrometry

Domenick, Taylor M. / Jones, Austin L. / Kemperman, Robin H. J. / Yost, Richard A.

Analytical and bioanalytical chemistry. 2022 July, v. 414, no. 18

2022

Abstract: The vast majority of mass spectrometry (MS)-based metabolomics studies employ reversed-phase liquid chromatography (RPLC) to separate analytes prior to MS detection. Highly polar metabolites, such as amino acids (AAs), are poorly retained by RPLC, making ...

Abstract	The vast majority of mass spectrometry (MS)-based metabolomics studies employ reversed-phase liquid chromatography (RPLC) to separate analytes prior to MS detection. Highly polar metabolites, such as amino acids (AAs), are poorly retained by RPLC, making quantitation of these key species challenging across the broad concentration ranges typically observed in biological specimens, such as cell extracts. To improve the detection and quantitation of AAs in microglial cell extracts, the implementation of a 4-dimethylaminobenzoylamido acetic acid N-hydroxysuccinimide ester (DBAA-NHS) derivatization agent was explored for its ability to improve both analyte retention and detection limits in RPLC-MS. In addition to the introduction of the DBAA-NHS labeling reagent, a uniformly (U) ¹³C-labeled yeast extract was also introduced during the sample preparation workflow as an internal standard (IS) to eliminate artifacts and to enable targeted quantitation of AAs, as well as untargeted amine submetabolome profiling. To improve method sensitivity and selectivity, multiplexed drift-tube ion mobility (IM) was integrated into the LC-MS workflow, facilitating the separation of isomeric metabolites, and improving the structural identification of unknown metabolites. Implementation of the U-¹³C-labeled yeast extract during the multiplexed LC-IM-MS analysis enabled the quantitation of 19 of the 20 common AAs, supporting a linear dynamic range spanning up to three orders of magnitude in concentration for microglial cell extracts, in addition to reducing the required cell count for reliable quantitation from 10 to 5 million cells per sample.
Keywords	acetic acid ; amino acids ; analytical chemistry ; chemical species ; derivatization ; mass spectrometry ; metabolites ; metabolomics ; neuroglia ; reversed-phase liquid chromatography ; yeast extract
Language	English
Dates of publication	2022-07
Size	p. 5549-5559.
Publishing place	Springer Berlin Heidelberg
Document type	Article
ISSN	1618-2642
DOI	10.1007/s00216-022-03993-w
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Article ; Online: Design and Implementation of a Dual-Probe Microsampling Apparatus for the Direct Analysis of Adherent Mammalian Cells by Ion Mobility-Mass Spectrometry.

Domenick, Taylor M / Vedam-Mai, Vinata / Yost, Richard A

Analytical chemistry

2020 Volume 92, Issue 17, Page(s) 12055–12061

Abstract: Atmospheric pressure sampling mass spectrometric methods are ideal platforms for rapidly analyzing the metabolomes of biological specimens. Several liquid extraction-based techniques have been developed for increasing metabolome coverage in direct ... ...

Abstract	Atmospheric pressure sampling mass spectrometric methods are ideal platforms for rapidly analyzing the metabolomes of biological specimens. Several liquid extraction-based techniques have been developed for increasing metabolome coverage in direct sampling workflows. Here, we report the construction of a dual-probe microsampling device (DPM), based on the design of the liquid microjunction surface sampling probe, for analyzing the metabolome of live microglial cells by drift-tube ion mobility spectrometry (IMS) quadrupole time-of-flight mass spectrometry. Utilizing two distinct solvent systems in parallel is demonstrated to extract a wide structural variety of metabolites and lipids, enabling a more comprehensive analysis of intracellular metabolism. Employing the DPM-IM-MS method to adherent cells yielded the detection of 73 unique lipids and 79 small molecule metabolites from each optimized solvent system probe, respectively. Integration of multiplexed ion mobility scans is also shown to increase extracted analyte signal intensities between 2- and 10-fold compared to traditional single-pulse IMS, enabling the detection of 38 low-intensity features not previously detected by single-pulse DPM-IM-MS. To examine the ability of the DPM system to differentiate between sample treatment groups, microglia were stimulated with the endotoxin lipopolysaccharide (LPS). Several metabolic alterations were detected between sample treatment groups by DPM-IM-MS, many of which were not previously detected with conventional single-probe liquid microjunction surface sampling.
MeSH term(s)	Animals ; Ion Mobility Spectrometry/methods ; Mass Spectrometry/methods ; Metabolomics/methods
Language	English
Publishing date	2020-08-20
Publishing country	United States
Document type	Journal Article ; Research Support, N.I.H., Extramural ; Research Support, Non-U.S. Gov't
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.0c02714
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Article ; Online: A rapid and robust method for amino acid quantification using a simple N-hydroxysuccinimide ester derivatization and liquid chromatography-ion mobility-mass spectrometry.

Domenick, Taylor M / Jones, Austin L / Kemperman, Robin H J / Yost, Richard A

Analytical and bioanalytical chemistry

2022 Volume 414, Issue 18, Page(s) 5549–5559

Abstract	The vast majority of mass spectrometry (MS)-based metabolomics studies employ reversed-phase liquid chromatography (RPLC) to separate analytes prior to MS detection. Highly polar metabolites, such as amino acids (AAs), are poorly retained by RPLC, making quantitation of these key species challenging across the broad concentration ranges typically observed in biological specimens, such as cell extracts. To improve the detection and quantitation of AAs in microglial cell extracts, the implementation of a 4-dimethylaminobenzoylamido acetic acid N-hydroxysuccinimide ester (DBAA-NHS) derivatization agent was explored for its ability to improve both analyte retention and detection limits in RPLC-MS. In addition to the introduction of the DBAA-NHS labeling reagent, a uniformly (U)
MeSH term(s)	Amines ; Amino Acids/analysis ; Chromatography, Liquid/methods ; Esters ; Mass Spectrometry/methods ; Metabolomics/methods ; Succinimides
Chemical Substances	Amines ; Amino Acids ; Esters ; Succinimides ; N-hydroxysuccinimide (MJE3791M4T)
Language	English
Publishing date	2022-03-26
Publishing country	Germany
Document type	Journal Article
ZDB-ID	201093-8
ISSN	1618-2650 ; 0016-1152 ; 0372-7920
ISSN (online)	1618-2650
ISSN	0016-1152 ; 0372-7920
DOI	10.1007/s00216-022-03993-w
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Article ; Online: Segmented Flow Strategies for Integrating Liquid Chromatography-Mass Spectrometry with Nuclear Magnetic Resonance for Lipidomics.

Lei, Jiajun / Mahar, Rohit / Chang, Mario C / Collins, James / Merritt, Matthew E / Garrett, Timothy J / Yost, Richard A

Analytical chemistry

2023

Abstract	Building an accurate lipid inventory relies on coordinated information from orthogonal analytical capabilities. Integrating the familiar workflow of liquid chromatography (LC), high-resolution mass spectrometry (HRMS), and tandem mass spectrometry (MS/MS) with proton nuclear magnetic resonance spectroscopy (
Language	English
Publishing date	2023-01-11
Publishing country	United States
Document type	Journal Article
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.2c03974
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Article ; Online: Per- and polyfluoroalkyl substances (PFAS) in sediments collected from the Pensacola Bay System watershed.

Ahmadireskety, Atiye / Da Silva, Bianca F / Awkerman, Jill A / Aufmuth, Joe / Yost, Richard A / Bowden, John A

Environmental advances

2023 Volume 5, Page(s) 1–8

Abstract: Sediment samples from 25 locations in the Pensacola Bay System (PBS) watershed were analyzed for the presence of 51 per- and polyfluoroalkyl substances (PFAS) using ultra high-performance liquid chromatography tandem mass spectrometry (UHPLC-MS/MS) and ... ...

Abstract	Sediment samples from 25 locations in the Pensacola Bay System (PBS) watershed were analyzed for the presence of 51 per- and polyfluoroalkyl substances (PFAS) using ultra high-performance liquid chromatography tandem mass spectrometry (UHPLC-MS/MS) and selected reaction monitoring. Results revealed quantifiable concentrations of PFAS in all sampling locations. More specifically, perfluorobutanoic acid (PFBA) was present in every sediment sample with a minimum and maximum concentration of 0.04 to 0.48 ng g
Language	English
Publishing date	2023-12-29
Publishing country	England
Document type	Journal Article
ISSN	2666-7657
ISSN (online)	2666-7657
DOI	10.1016/j.envadv.2021.100088
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Article ; Online: Metabolomic and Lipidomic Characterization of Meningioma Grades Using LC-HRMS and Machine Learning.

Safari Yazd, Hoda / Bazargani, Sina Feizbakhsh / Fitzpatrick, Garrett / Yost, Richard A / Kresak, Jesse / Garrett, Timothy J

Journal of the American Society for Mass Spectrometry

2023 Volume 34, Issue 10, Page(s) 2187–2198

Abstract: Meningiomas are among the most common brain tumors that arise from the leptomeningeal cover of the brain and spinal cord and account for around 37% of all central nervous system tumors. According to the World Health Organization, meningiomas are ... ...

Abstract	Meningiomas are among the most common brain tumors that arise from the leptomeningeal cover of the brain and spinal cord and account for around 37% of all central nervous system tumors. According to the World Health Organization, meningiomas are classified into three histological subtypes: benign, atypical, and anaplastic. Sometimes, meningiomas with a histological diagnosis of benign tumors show clinical characteristics and behavior of aggressive tumors. In this study, we examined the metabolomic and lipidomic profiles of meningioma tumors, focusing on comparing low-grade and high-grade tumors and identifying potential markers that can discriminate between benign and malignant tumors. High-resolution mass spectrometry coupled to liquid chromatography was used for untargeted metabolomics and lipidomics analyses of 85 tumor biopsy samples with different meningioma grades. We then applied feature selection and machine learning techniques to find the features with the highest information to aid in the diagnosis of meningioma grades. Three biomarkers were identified to differentiate low- and high-grade meningioma brain tumors. The use of mass-spectrometry-based metabolomics and lipidomics combined with machine learning analyses to prospect and characterize biomarkers associated with meningioma grades may pave the way for elucidating potential therapeutic and prognostic targets.
MeSH term(s)	Humans ; Meningioma/diagnosis ; Meningioma/pathology ; Meningeal Neoplasms/diagnosis ; Meningeal Neoplasms/pathology ; Lipidomics ; Brain Neoplasms/diagnosis ; Biomarkers ; Machine Learning
Chemical Substances	Biomarkers
Language	English
Publishing date	2023-09-14
Publishing country	United States
Document type	Journal Article
ZDB-ID	1073671-2
ISSN	1879-1123 ; 1044-0305
ISSN (online)	1879-1123
ISSN	1044-0305
DOI	10.1021/jasms.3c00158
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Zs.MO 241: Show issues

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