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Metabolites
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Advances in Ambient Ionization Techniques for Mass Spectrometry
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Advances in Ambient Ionization Techniques for Mass Spectrometry

A special issue of Metabolites (ISSN 2218-1989). This special issue belongs to the section "Cell Metabolism".

Deadline for manuscript submissions: closed (1 October 2021) | Viewed by 30178

Special Issue Editors

Prof. Dr. Peter Oefner

E-Mail Website
Guest Editor
Institute of Functional Genomics, University of Regensburg, Am BioPark 9, 93053 Regensburg, Germany
Interests: NMR- and MS-based metabolomics; cancer and immune cell metabolism; chronic kidney disease; gut microbiota and immunity; bioinformatics
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Zoltan Takats

E-Mail Website
Guest Editor
Head of Division of Systems Medicine, Department of Metabolism, Digestion and Reproduction, Imperial College London, London SW7 2AZ, UK
Interests: analytical chemistry; Mass Spectrometry; cancer research
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In 2004, solvent-based desorption electrospray ionization (DESI) was the first ambient ionization technique to be introduced and applied to the direct and real-time analysis of small and large compounds with little or no sample pretreatment in their native environment. To date, more than twenty methods have been described for the effective desorption and ionization of molecules under ambient conditions, ranging from liquid to plasma, laser, thermal, vibrational, acoustic, and evaporative desorption. Continued technical refinement has resulted in steadily improved analytical reproducibility, spatial resolution, detection sensitivity and analyte coverage, the latter having been spurred by advances in ion mobility spectrometry and on-substrate derivatization. Applications include tissue imaging, single cell analysis, therapeutic drug monitoring, in vivo analysis, forensics, reaction monitoring and catalysis, and food testing. The planned Special Issue invites both original and review articles on both technical and methodological developments, as well as applications of ambient ionization mass spectrometry to the analysis of metabolites, lipids and peptides. The submission deadline is 1 October 2021.

Prof. Dr. Peter Oefner
Prof. Dr. Zoltan Takats
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Metabolites is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • ambient ionization techniques
  • imaging mass spectrometry
  • on-substrate derivatizationpoint-of-care testing
  • reaction monitoring
  • microbial profiling
  • in-vivo analysis

Published Papers (11 papers)

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Research

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11 pages, 2533 KiB  
Article
Direct In Vivo Analysis of CBD- and THC-Acid Cannabinoids and Classification of Cannabis Cultivars Using SpiderMass
by Nina Ogrinc, Serge Schneider, Adèle Bourmaud, Nicolas Gengler, Michel Salzet and Isabelle Fournier
Metabolites 2022, 12(6), 480; https://doi.org/10.3390/metabo12060480 - 26 May 2022
Cited by 1 | Viewed by 1935
Abstract
In recent years, cannabis and hemp-based products have become increasingly popular for recreational use, edibles, beverages, health care products, and medicines. The rapid detection and differentiation of phytocannabinoids is, therefore, essential to assess the potency and the therapeutic and nutritional values of cannabis [...] Read more.
In recent years, cannabis and hemp-based products have become increasingly popular for recreational use, edibles, beverages, health care products, and medicines. The rapid detection and differentiation of phytocannabinoids is, therefore, essential to assess the potency and the therapeutic and nutritional values of cannabis cultivars. Here, we implemented SpiderMass technology for in vivo detection of cannabidiolic acid (CBDA) and ∆9-tetrahydrocannabinolicacid (∆9-THCA), and other endogenous organic plant compounds, to access distribution gradients within the plants and differentiate between cultivars. The SpiderMass system is composed of an IR-laser handheld microsampling probe connected to a mass spectrometer through a transfer tube. The analysis was performed on different plant organs from freshly cultivated cannabis plants in only a few seconds. SpiderMass analysis easily discriminated the two acid phytocannabinoid isomers via MS/MS, and the built statistical models differentiated between four cannabis cultivars. Different abundancies of the two acid phytocannabinoids were found along the plant as well as between different cultivars. Overall, these results introduce direct analysis by SpiderMass as a compelling analytical alternative for rapid hemp analysis. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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15 pages, 1830 KiB  
Article
Automated Cancer Diagnostics via Analysis of Optical and Chemical Images by Deep and Shallow Learning
by Olof Gerdur Isberg, Valentina Giunchiglia, James S. McKenzie, Zoltan Takats, Jon Gunnlaugur Jonasson, Sigridur Klara Bodvarsdottir, Margret Thorsteinsdottir and Yuchen Xiang
Metabolites 2022, 12(5), 455; https://doi.org/10.3390/metabo12050455 - 18 May 2022
Viewed by 2903
Abstract
Optical microscopy has long been the gold standard to analyse tissue samples for the diagnostics of various diseases, such as cancer. The current diagnostic workflow is time-consuming and labour-intensive, and manual annotation by a qualified pathologist is needed. With the ever-increasing number of [...] Read more.
Optical microscopy has long been the gold standard to analyse tissue samples for the diagnostics of various diseases, such as cancer. The current diagnostic workflow is time-consuming and labour-intensive, and manual annotation by a qualified pathologist is needed. With the ever-increasing number of tissue blocks and the complexity of molecular diagnostics, new approaches have been developed as complimentary or alternative solutions for the current workflow, such as digital pathology and mass spectrometry imaging (MSI). This study compares the performance of a digital pathology workflow using deep learning for tissue recognition and an MSI approach utilising shallow learning to annotate formalin-fixed and paraffin-embedded (FFPE) breast cancer tissue microarrays (TMAs). Results show that both deep learning algorithms based on conventional optical images and MSI-based shallow learning can provide automated diagnostics with F1-scores higher than 90%, with the latter intrinsically built on biochemical information that can be used for further analysis. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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14 pages, 3683 KiB  
Article
Correlating Mass Spectrometry Imaging and Liquid Chromatography-Tandem Mass Spectrometry for Tissue-Based Pharmacokinetic Studies
by Andreas Dannhorn, Emine Kazanc, Gregory Hamm, John G. Swales, Nicole Strittmatter, Gareth Maglennon, Richard J. A. Goodwin and Zoltan Takats
Metabolites 2022, 12(3), 261; https://doi.org/10.3390/metabo12030261 - 18 Mar 2022
Cited by 4 | Viewed by 2787
Abstract
Liquid chromatography-tandem mass spectrometry (LC-MS/MS) is a standard tool used for absolute quantification of drugs in pharmacokinetic (PK) studies. However, all spatial information is lost during the extraction and elucidation of a drugs biodistribution within the tissue is impossible. In the study presented [...] Read more.
Liquid chromatography-tandem mass spectrometry (LC-MS/MS) is a standard tool used for absolute quantification of drugs in pharmacokinetic (PK) studies. However, all spatial information is lost during the extraction and elucidation of a drugs biodistribution within the tissue is impossible. In the study presented here we used a sample embedding protocol optimized for mass spectrometry imaging (MSI) to prepare up to 15 rat intestine specimens at once. Desorption electrospray ionization (DESI) and matrix assisted laser desorption/ionization (MALDI) mass spectrometry imaging (MSI) were employed to determine the distributions and relative abundances of four benchmarking compounds in the intestinal segments. High resolution MALDI-MSI experiments performed at 10 µm spatial resolution allowed to determine the drug distribution in the different intestinal histological compartments to determine the absorbed and tissue bound fractions of the drugs. The low tissue bound drug fractions, which were determined to account for 56–66% of the total drug, highlight the importance to understand the spatial distribution of drugs within the histological compartments of a given tissue to rationalize concentration differences found in PK studies. The mean drug abundances of four benchmark compounds determined by MSI were correlated with the absolute drug concentrations. Linear regression resulted in coefficients of determination (R2) ranging from 0.532 to 0.926 for MALDI-MSI and R2 values ranging from 0.585 to 0.945 for DESI-MSI, validating a quantitative relation of the imaging data. The good correlation of the absolute tissue concentrations of the benchmark compounds and the MSI data provides a bases for relative quantification of compounds within and between tissues, without normalization to an isotopically labelled standard, provided that the compared tissues have inherently similar ion suppression effects. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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14 pages, 4823 KiB  
Article
Enhancing Metabolomic Coverage in Positive Ionization Mode Using Dicationic Reagents by Infrared Matrix-Assisted Laser Desorption Electrospray Ionization
by Ying Xi and David C. Muddiman
Metabolites 2021, 11(12), 810; https://doi.org/10.3390/metabo11120810 - 29 Nov 2021
Cited by 1 | Viewed by 1838
Abstract
Mass spectrometry imaging is a powerful tool to analyze a large number of metabolites with their spatial coordinates collected throughout the sample. However, the significant differences in ionization efficiency pose a big challenge to metabolomic mass spectrometry imaging. To solve the challenge and [...] Read more.
Mass spectrometry imaging is a powerful tool to analyze a large number of metabolites with their spatial coordinates collected throughout the sample. However, the significant differences in ionization efficiency pose a big challenge to metabolomic mass spectrometry imaging. To solve the challenge and obtain a complete data profile, researchers typically perform experiments in both positive and negative ionization modes, which is time-consuming. In this work, we evaluated the use of the dicationic reagent, 1,5-pentanediyl-bis(1-butylpyrrolidinium) difluoride (abbreviated to [C5(bpyr)2]F2) to detect a broad range of metabolites in the positive ionization mode by infrared matrix-assisted laser desorption electrospray ionization mass spectrometry imaging (IR-MALDESI MSI). [C5(bpyr)2]F2 at 10 µM was doped in 50% MeOH/H2O (v/v) electrospray solvent to form +1 charged adducted ions with anionic species (−1 charged) through post-electrospray ionization. This method was demonstrated with sectioned rat liver and hen ovary. A total of 73 deprotonated metabolites from rat liver tissue sections were successfully adducted with [C5(bpyr)2]2+ and putatively identified in the adducted positive ionization polarity, along with 164 positively charged metabolite ions commonly seen in positive ionization mode, which resulted in 44% increased molecular coverage. In addition, we were able to generate images of hen ovary sections showing their morphological features. Following-up tandem mass spectrometry (MS/MS) indicated that this dicationic reagent [C5(bpyr)2]2+ could form ionic bonds with the headgroup of glycerophospholipid ions. The addition of the dicationic reagent [C5(bpyr)2]2+ in the electrospray solvent provides a rapid and effective way to enhance the detection of metabolites in positive ionization mode. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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11 pages, 3449 KiB  
Article
High-Throughput Analysis from Complex Matrices: Acoustic Ejection Mass Spectrometry from Phase-Separated Fluid Samples
by Yuzhu Guo, Michael Forbush, Thomas R. Covey, Lucien Ghislain and Chang Liu
Metabolites 2021, 11(11), 789; https://doi.org/10.3390/metabo11110789 - 18 Nov 2021
Cited by 11 | Viewed by 2049
Abstract
Acoustic ejection mass spectrometry is a novel high-throughput analytical technology that delivers high reproducibility without carryover observed. It eliminates the chromatography step used to separate analytes from matrix components. Fully-automated liquid–liquid extraction is widely used for sample cleanup, especially in high-throughput applications. We [...] Read more.
Acoustic ejection mass spectrometry is a novel high-throughput analytical technology that delivers high reproducibility without carryover observed. It eliminates the chromatography step used to separate analytes from matrix components. Fully-automated liquid–liquid extraction is widely used for sample cleanup, especially in high-throughput applications. We introduce a workflow for direct AEMS analysis from phase-separated liquid samples and explore high-throughput analysis from complex matrices. We demonstrate the quantitative determination of fentanyl from urine using this two-phase AEMS approach, with a LOD lower than 1 ng/mL, quantitation precision of 15%, and accuracy better than ±10% over the range of evaluation (1–100 ng/mL). This workflow offers simplified sample preparation and higher analytical throughput for some bioanalytical applications, in comparison to an LC-MS based approach. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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10 pages, 800 KiB  
Article
The Impact of Histological Annotations for Accurate Tissue Classification Using Mass Spectrometry Imaging
by Juliana Pereira Lopes Gonçalves, Christine Bollwein, Anna Melissa Schlitter, Benedikt Martin, Bruno Märkl, Kirsten Utpatel, Wilko Weichert and Kristina Schwamborn
Metabolites 2021, 11(11), 752; https://doi.org/10.3390/metabo11110752 - 30 Oct 2021
Cited by 6 | Viewed by 2163
Abstract
Knowing the precise location of analytes in the tissue has the potential to provide information about the organs’ function and predict its behavior. It is especially powerful when used in diagnosis and prognosis prediction of pathologies, such as cancer. Spatial proteomics, in particular [...] Read more.
Knowing the precise location of analytes in the tissue has the potential to provide information about the organs’ function and predict its behavior. It is especially powerful when used in diagnosis and prognosis prediction of pathologies, such as cancer. Spatial proteomics, in particular mass spectrometry imaging, together with machine learning approaches, has been proven to be a very helpful tool in answering some histopathology conundrums. To gain accurate information about the tissue, there is a need to build robust classification models. We have investigated the impact of histological annotation on the classification accuracy of different tumor tissues. Intrinsic tissue heterogeneity directly impacts the efficacy of the annotations, having a more pronounced effect on more heterogeneous tissues, as pancreatic ductal adenocarcinoma, where the impact is over 20% in accuracy. On the other hand, in more homogeneous samples, such as kidney tumors, histological annotations have a slenderer impact on the classification accuracy. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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13 pages, 2504 KiB  
Article
Distinguishing between Isobaric Ions Using Microdroplet Hydrogen–Deuterium Exchange Mass Spectrometry
by Xiaowei Song, Jia Li, Mohammad Mofidfar and Richard N. Zare
Metabolites 2021, 11(11), 728; https://doi.org/10.3390/metabo11110728 - 23 Oct 2021
Cited by 10 | Viewed by 2679
Abstract
Isobaric ions having the same mass-to-charge ratio cannot be separately identified by mass spectrometry (MS) alone, but this limitation can be overcome by using hydrogen–deuterium exchange (HDX) in microdroplets. Because isobaric ions may contain a varied number of exchangeable sites and different types [...] Read more.
Isobaric ions having the same mass-to-charge ratio cannot be separately identified by mass spectrometry (MS) alone, but this limitation can be overcome by using hydrogen–deuterium exchange (HDX) in microdroplets. Because isobaric ions may contain a varied number of exchangeable sites and different types of functional groups, each one produces a unique MS spectral pattern after droplet spray HDX without the need for MS/MS experiments or introduction of ion mobility measurements. As an example of the power of this approach, isobaric ions in urinary metabolic profiles are identified and used to distinguish between healthy individuals and those having bladder cancer. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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13 pages, 3174 KiB  
Article
Matrix-Free High-Resolution Atmospheric-Pressure SALDI Mass Spectrometry Imaging of Biological Samples Using Nanostructured DIUTHAME Membranes
by Max A. Müller, Dhaka R. Bhandari and Bernhard Spengler
Metabolites 2021, 11(9), 624; https://doi.org/10.3390/metabo11090624 - 15 Sep 2021
Cited by 5 | Viewed by 3110
Abstract
Applications of mass spectrometry imaging (MSI), especially matrix-assisted laser desorption/ionization (MALDI) in the life sciences are becoming increasingly focused on single cell analysis. With the latest instrumental developments, pixel sizes in the micrometer range can be obtained, leading to challenges in matrix application, [...] Read more.
Applications of mass spectrometry imaging (MSI), especially matrix-assisted laser desorption/ionization (MALDI) in the life sciences are becoming increasingly focused on single cell analysis. With the latest instrumental developments, pixel sizes in the micrometer range can be obtained, leading to challenges in matrix application, where imperfections or inhomogeneities in the matrix layer can lead to misinterpretation of MS images. Thereby, the application of premanufactured, homogeneous ionization-assisting devices is a promising approach. Tissue sections were investigated using a matrix-free imaging technique (Desorption Ionization Using Through-Hole Alumina Membrane, DIUTHAME) based on premanufactured nanostructured membranes to be deposited on top of a tissue section, in comparison to the spray-coating of an organic matrix in a MALDI MSI approach. Atmospheric pressure MALDI MSI ion sources were coupled to orbital trapping mass spectrometers. MS signals obtained by the different ionization techniques were annotated using accurate-mass-based database research. Compared to MALDI MSI, DIUTHAME MS images captivated with higher signal homogeneities, higher contrast and reduced background signals, while signal intensities were reduced by about one order of magnitude, independent of analyte class. DIUTHAME membranes, being applicable only on tissue sections thicker than 50 µm, were successfully used for mammal, insect and plant tissue with a high lateral resolution down to 5 µm. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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Review

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18 pages, 3080 KiB  
Review
Review of Recent Advances in Lipid Analysis of Biological Samples via Ambient Ionization Mass Spectrometry
by Haiyan Lu, Hua Zhang, Shuling Xu and Lingjun Li
Metabolites 2021, 11(11), 781; https://doi.org/10.3390/metabo11110781 - 15 Nov 2021
Cited by 9 | Viewed by 3835
Abstract
The rapid and direct structural characterization of lipids proves to be critical for studying the functional roles of lipids in many biological processes. Among numerous analytical techniques, ambient ionization mass spectrometry (AIMS) allows for a direct molecular characterization of lipids from various complex [...] Read more.
The rapid and direct structural characterization of lipids proves to be critical for studying the functional roles of lipids in many biological processes. Among numerous analytical techniques, ambient ionization mass spectrometry (AIMS) allows for a direct molecular characterization of lipids from various complex biological samples with no/minimal sample pretreatment. Over the recent years, researchers have expanded the applications of the AIMS techniques to lipid structural elucidation via a combination with a series of derivatization strategies (e.g., the Paternò–Büchi (PB) reaction, ozone-induced dissociation (OzID), and epoxidation reaction), including carbon–carbon double bond (C=C) locations and sn-positions isomers. Herein, this review summarizes the reaction mechanisms of various derivatization strategies for C=C bond analysis, typical instrumental setup, and applications of AIMS in the structural elucidation of lipids from various biological samples (e.g., tissues, cells, and biofluids). In addition, future directions of AIMS for lipid structural elucidation are discussed. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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22 pages, 4452 KiB  
Review
Recent Advances of Ambient Mass Spectrometry Imaging and Its Applications in Lipid and Metabolite Analysis
by Keke Qi, Liutian Wu, Chengyuan Liu and Yang Pan
Metabolites 2021, 11(11), 780; https://doi.org/10.3390/metabo11110780 - 15 Nov 2021
Cited by 18 | Viewed by 2834
Abstract
Ambient mass spectrometry imaging (AMSI) has attracted much attention in recent years. As a kind of unlabeled molecular imaging technique, AMSI can enable in situ visualization of a large number of compounds in biological tissue sections in ambient conditions. In this review, the [...] Read more.
Ambient mass spectrometry imaging (AMSI) has attracted much attention in recent years. As a kind of unlabeled molecular imaging technique, AMSI can enable in situ visualization of a large number of compounds in biological tissue sections in ambient conditions. In this review, the developments of various AMSI techniques are discussed according to one-step and two-step ionization strategies. In addition, recent applications of AMSI for lipid and metabolite analysis (from 2016 to 2021) in disease diagnosis, animal model research, plant science, drug metabolism and toxicology research, etc., are summarized. Finally, further perspectives of AMSI in spatial resolution, sensitivity, quantitative ability, convenience and software development are proposed. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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Other

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17 pages, 18047 KiB  
Perspective
Build, Share and Remix: 3D Printing for Speeding Up the Innovation Cycles in Ambient Ionisation Mass Spectrometry (AIMS)
by Nancy Shyrley García-Rojas, Héctor Guillén-Alonso, Sandra Martínez-Jarquín, Abigail Moreno-Pedraza, Leonardo D. Soto-Rodríguez and Robert Winkler
Metabolites 2022, 12(2), 185; https://doi.org/10.3390/metabo12020185 - 17 Feb 2022
Cited by 4 | Viewed by 2557
Abstract
Ambient ionisation mass spectrometry (AIMS) enables studying biological systems in their native state and direct high-throughput analyses. The ionisation occurs in the physical conditions of the surrounding environment. Simple spray or plasma-based AIMS devices allow the desorption and ionisation of molecules from solid, [...] Read more.
Ambient ionisation mass spectrometry (AIMS) enables studying biological systems in their native state and direct high-throughput analyses. The ionisation occurs in the physical conditions of the surrounding environment. Simple spray or plasma-based AIMS devices allow the desorption and ionisation of molecules from solid, liquid and gaseous samples. 3D printing helps to implement new ideas and concepts in AIMS quickly. Here, we present examples of 3D printed AIMS sources and devices for ion transfer and manipulation. Further, we show the use of 3D printer parts for building custom AIMS sampling robots and imaging systems. Using 3D printing technology allows upgrading existing mass spectrometers with relatively low cost and effort. Full article
(This article belongs to the Special Issue Advances in Ambient Ionization Techniques for Mass Spectrometry)
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