Deeper Understanding of Solvent-Based Ambient Ionization Mass Spectrometry: Are Molecular Profiles Primarily Dictated by Extraction Mechanisms?

Lin, Monica; Blevins, Molly S.; Sans, Marta; Brodbelt, Jennifer S.; Eberlin, Lívia S.

doi:10.1021/acs.analchem.2c03360

Cited by 7 publications

(4 citation statements)

References 53 publications

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“…Chemical and mass spectral information (including MS/MS transitions) for each NAM is displayed in Table S1. As is typical for many spray‐based, ambient MS ionization sources, 39,42,43 collected spectra for both PSI‐MS and FCSI‐MS are highly simplistic, predominantly exhibiting protonated molecular ions for the target NAMs. Representative PSI‐MS and MS/MS spectra are shown in Figure 1, collected from 200 ng residues of individual NAMs deposited onto a paper substrate.…”

Section: Resultsmentioning

confidence: 99%

Rapid screening of high‐priority N‐nitrosamines in pharmaceutical, forensic, and environmental samples with paper spray ionization and filter cone spray ionization‐mass spectrometry

McDaniel

Holtz

Bondzie

et al. 2023

Rapid Comm Mass Spectrometry

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RationaleThe burgeoning concern of N‐nitrosamine (NAM) contamination found in various pharmaceutical compositions has increased the demand for rapid and reliable screening methods to better assess the breadth of the problem. These carcinogenic compounds are also found in food, water, and soil, and they have been used in poison‐related homicides.MethodsA combination of complementary, ambient ionization methods, paper spray ionization (PSI) and filter cone spray ionization (FCSI)‐mass spectrometry (MS), was characterized towards trace‐level residue screening of select NAMs (e.g., N‐nitrosodimethylamine, N‐nitrosodiethylamine, N‐nitrosodibutylamine) directly from complex and problematic matrices of interest, including prescription and over‐the‐counter tablets, drinking water, soil, and consumable goods. Spectral data for analyte confirmation and detection limit studies were collected using a Thermo LCQ Fleet ion trap mass spectrometer.ResultsPSI‐MS and FCSI‐MS readily produced mass spectral data marked by their simplicity (e.g., predominantly protonated molecular ions observed) and congruence with traditional electrospray ionization mass spectra in under 2 min. per sample. Both methods proved robust to the complex matrices tested, yielding ion signatures for target NAMs, as well as active pharmaceutical ingredients for analyzed tablets, flavorants inherent to food products, etc. Low part‐per‐million detection limits were observed but were shown dependent on sample composition.ConclusionsPSI‐MS and FCSI‐MS were successful in detecting trace‐level NAMS in complex liquid‐ and solid‐phase matrices with little to no prior preparation. This work suggests that these methodologies can provide a means for assessing problematic pharmaceutical adulterants/degradants for expedited quality control, as well as enhancing environmental stewardship efforts and forensic investigations.

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Section: Resultsmentioning

confidence: 99%

Rapid screening of high‐priority N‐nitrosamines in pharmaceutical, forensic, and environmental samples with paper spray ionization and filter cone spray ionization‐mass spectrometry

McDaniel

Holtz

Bondzie

et al. 2023

Rapid Comm Mass Spectrometry

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“…Differences in the mass spectral profiles were also observed when comparing data obtained with ACN:DMF and MeOH solvents on the same MS platform, with the most notable difference being higher relative abundance of CLs using ACN:DMF and a higher relative abundance of PEs in MeOH (Figure , Supporting Information). There are many factors that could be playing a role in these observed mass spectral differences, including differences in extraction efficiency of different lipids in the different solvent systems, physicochemical properties of the solvents, and differences in ionization efficiencies …”

Section: Resultsmentioning

confidence: 99%

“…There are many factors that could be playing a role in these observed mass spectral differences, including differences in extraction efficiency of different lipids in the different solvent systems, physicochemical properties of the solvents, and differences in ionization efficiencies. 11 We next used a statistical classifier previously developed from DESI-MS imaging data acquired on an orbitrap using ACN:DMF solvent for discriminating PTC from benign thyroid tumors to predict on the m-FNA data obtained under the different conditions in this study. 3 The classifier, built using logistic regression in combination with lasso regularization, 12 is comprised of 67 m/z features, 3 (PS 38:2), heavily weighted toward PTC.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Evaluating the Generalizability of Predictive Classifiers Built from DESI Imaging Lipid Data across Mass Spectrometry Platforms

DeHoog

Lin

Roman

et al. 2023

J. Am. Soc. Mass Spectrom.

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In this study, we evaluate the generalizability of predictive classifiers built from DESI lipid data for thyroid fine needle aspiration (FNA) biopsy analysis and classification using two high-performance mass spectrometers (time-of-flight and orbitrap) suited with different DESI imaging sources operated by different users. The molecular profiles obtained from thyroid samples with the different platforms presented similar trends, although specific differences in ion abundances were observed. When using a previously published statistical model built to discriminate thyroid cancer from benign thyroid tissues to predict on a new independent data set obtained, agreement for 24 of the 30 samples across the imaging platforms was achieved. We also tested the classifier on six clinical FNAs and obtained agreement between the predictive results and clinical diagnosis for the different conditions. Altogether, our results provide evidence that statistical classifiers generated from DESI lipid data are applicable across different high-resolution mass spectrometry platforms for thyroid FNA classification.

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“…performed an evaluation of the effects of different solvent systems and extraction times on the extraction and detection of different molecules. 185 Chemical profiles were notably affected by the use of different solvent systems and extraction times, highlighting the importance of extensive optimization when developing solvent‐based AIMS techniques. Krenkel et al.…”

Section: Applications Of Aimsmentioning

confidence: 99%

Applications of ambient ionization mass spectrometry in 2022: An annual review

Rankin‐Turner

Sears

Heaney

2023

Analytical Science Advances

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The development of ambient ionization mass spectrometry (AIMS) has transformed analytical science, providing the means of performing rapid analysis of samples in their native state, both in and out of the laboratory. The capacity to eliminate sample preparation and pre‐MS separation techniques, leading to true real‐time analysis, has led to AIMS naturally gaining a broad interest across the scientific community. Since the introduction of the first AIMS techniques in the mid‐2000s, the field has exploded with dozens of novel ion sources, an array of intriguing applications, and an evident growing interest across diverse areas of study. As the field continues to surge forward each year, ambient ionization techniques are increasingly becoming commonplace in laboratories around the world. This annual review provides an overview of AIMS techniques and applications throughout 2022, with a specific focus on some of the major fields of research, including forensic science, disease diagnostics, pharmaceuticals and food sciences. New techniques and methods are introduced, demonstrating the unwavering drive of the analytical community to further advance this exciting field and push the boundaries of what analytical chemistry can achieve.

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Deeper Understanding of Solvent-Based Ambient Ionization Mass Spectrometry: Are Molecular Profiles Primarily Dictated by Extraction Mechanisms?

Cited by 7 publications

References 53 publications

Rapid screening of high‐priority N‐nitrosamines in pharmaceutical, forensic, and environmental samples with paper spray ionization and filter cone spray ionization‐mass spectrometry

Rapid screening of high‐priority N‐nitrosamines in pharmaceutical, forensic, and environmental samples with paper spray ionization and filter cone spray ionization‐mass spectrometry

Evaluating the Generalizability of Predictive Classifiers Built from DESI Imaging Lipid Data across Mass Spectrometry Platforms

Applications of ambient ionization mass spectrometry in 2022: An annual review

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