Review
Biochemical Research Methods
Lanaia Itala Louzeiro Maciel, Ricardo Alves Bernardo, Rafael Oliveira Martins, Almir Custodio Batista Jr, Joao Victor Ataide Oliveira, Andrea Rodrigues Chaves, Boniek Gontijo Vaz
Summary: The imaging of biological tissues using mass spectrometry imaging (MSI) techniques allows for the visualization of the distribution of various metabolites, drugs, lipids, and glycans in complex samples. MSI methods like DESI-MSI and MALDI-MSI provide high sensitivity and the ability to evaluate/visualize multiple analytes in a single sample, overcoming limitations of classical microscopy techniques. This review discusses the application of DESI-MSI and MALDI-MSI in evaluating exogenous and endogenous molecules in biological samples, providing technical insights and recent research findings.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Article
Biochemical Research Methods
Alena N. Joignant, Hongxia Bai, Jacob P. Guymon, Kenneth P. Garrard, Mark Pankow, David C. Muddiman
Summary: This article presents the development and characterization of the NextGen infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) instrument, including the development of a new analysis geometry. The study demonstrates comparable results between vertically oriented transmission mode (tm)-IR-MALDESI and reflection mode (rm)-IR-MALDESI on mouse tissue. It also examines the use of glycerol as an alternative matrix, which shows little improvement in ion abundances for tm-IR-MALDESI.
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
(2022)
Article
Chemistry, Multidisciplinary
Ouyang Dan, Chuanzhe Wang, Chao Zhong, Juan Lin, Gang Xu, Guane Wang, Zian Lin
Summary: In this study, novel LDI-MS substrates were designed to enhance the sensitivity of mass signals and achieve high accuracy diagnosis of different saccharides and central precocious puberty (CPP).
Article
Chemistry, Analytical
Joseph H. H. Holbrook, Emily R. R. Sekera, Arbil Lopez, Brian D. D. Fries, Fernando Tobias, Kubra Akkaya, Maria M. M. Mihaylova, Amanda B. B. Hummon
Summary: Lipids are essential macromolecules that play crucial roles in numerous biological events. Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) is a powerful tool for understanding the spatial localization of lipids in biological systems. In this study, the use of ammonium fluoride (NH4F) as a comatrix additive was found to enhance lipid detection in biological samples, with a signal increase of up to 200%. The addition of NH4F was observed to enhance the lipid signal of [M-H](-) ions, attributed to a proton transfer reaction in various lipid classes. Overall, the study shows that the NH4F comatrix additive significantly improves sensitivity for lipid detection in a MALDI system and can be applied to various applications.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Frederic Fournelle, Nidia Lauzon, Ethan Yang, Pierre Chaurand
Summary: Traditionally, MALDI IMS requires the deposition of an organic matrix, which often generates high background noise in the low mass range. LDI offers selective ionization with low background in the low mass range. This article discusses the advantages and disadvantages of solvent free and wet deposition of metals as LDI matrices and demonstrates the power of metal-assisted LDI for analyzing low molecular weight molecules in tissue sections.
MICROCHEMICAL JOURNAL
(2023)
Article
Multidisciplinary Sciences
Hua Zhang, Lin Zhao, Jingjing Jiang, Jie Zheng, Li Yang, Yanyan Li, Jian Zhou, Tianshu Liu, Jianmin Xu, Wenhui Lou, Weige Yang, Lijie Tan, Weiren Liu, Yiyi Yu, Meiling Ji, Yaolin Xu, Yan Lu, Xiaomu Li, Zhen Liu, Rong Tian, Cheng Hu, Shumang Zhang, Qinsheng Hu, Yangdong Deng, Hao Ying, Sheng Zhong, Xingdong Zhang, Yunbing Wang, Hua Wang, Jingwei Bai, Xiaoying Li, Xiangfeng Duan
Summary: As cancer is increasingly seen as a metabolic disorder, serum metabolite profiling is proposed as a viable method for detecting cancer. In this study, a machine learning model using mass spectrometry-based liquid biopsy data is reported for pan-cancer screening and classification. The Multiplexed Nanomaterial-Assisted LDI for Cancer Identification (MNALCI) achieves high sensitivity and specificity for distinguishing cancers from healthy controls and accurately identifying the tissue of origin of tumors. This high throughput assay shows promising potential for non-invasive cancer diagnosis.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Paulina Kobylis, Marta Kasprzyk, Andrzej Nowacki, Magda Caban
Summary: This study tested the ionicity of selected ionic liquid matrices (ILMs) and their impact on the MALDI process, using various techniques for detection and analysis. It was found that HABA/alpha-MBA is a very good ionic liquid, while the ionicity of other matrices was reduced due to intermolecular interactions. Mass spectra analysis showed that the base peaks depended on amine gas proton affinity.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Physics, Atomic, Molecular & Chemical
Max D. Sharin, Gabriella M. Floro, Kevin D. Clark
Summary: Electrospray ionization (ESI) and matrix-assisted laser desorption ionization (MALDI) have revolutionized nucleic acid analysis by mass spectrometry. However, complex biological samples and large nucleic acids pose challenges for these techniques. Over the past two decades, innovations in sample preparation methods have been vital in overcoming these challenges and advancing high-throughput, sensitive, and broadly applicable MS methods for nucleic acid analysis.
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Maximilian Muhr, Patricia Heiss, Max Schuetz, Raphael Buehler, Christian Gemel, Mathias H. Linden, H. Bernhard Linden, Roland A. Fischer
Summary: The new setup combining a ThermoFisher Exactive Plus Orbitrap Mass Spectrometer with a LIFDI source allows for the analysis of sensitive organometallic complexes. The detection of oxygen traces and mass spectrometric analysis of Cu/Al cluster mixtures are successfully conducted using this setup.
DALTON TRANSACTIONS
(2021)
Article
Biochemical Research Methods
Juha-Pekka Hieta, Nina Sipari, Heikki Raikkonen, Markku Keinanen, Risto Kostiainen
Summary: This study demonstrates the potential of infrared laser ablation atmospheric pressure photoionization mass spectrometry (LAAPPI-MS) in analyzing the substructures of Arabidopsis thaliana leaves and its application in depth profiling analysis. The results show that LAAPPI-MS can detect variations in the distribution of various metabolites among different substructures of A. thaliana leaves.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Review
Chemistry, Analytical
Theoneste Muyizere, Janvier Mukiza
Summary: This review summarizes the application of metal ion-assisted ionization sources in the mass spectrometric analysis of polymers and discusses different ionization systems. It also provides an outlook on the future research trends and challenges in this field.
ANALYTICAL METHODS
(2022)
Article
Chemistry, Physical
Zixiang Wei, Jae Bem You, Hongbo Zeng, Xuehua Zhang
Summary: This work demonstrates that colorimetric chemical reactions in surface nanodroplets can alter the partitioning of acid analytes, resulting in increased acidity within the droplets. The distribution coefficient of the acid can be shifted by 3-11 times compared to the bulk solution. Such enhanced extraction and partitioning in droplets may be leveraged for highly sensitive chemical detection.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Biochemical Research Methods
Vishnu Shankar, Robert Tibshirani, Richard N. Zare
Summary: DESI-MSI has been increasingly used for detecting metabolites and lipids from human tissues and biofluids, but accurate computational and statistical methods are necessary to identify significant differences. MassExplorer is a flexible tool that helps researchers preprocess data, visualize structures, and select statistically significant metabolites.
Review
Chemistry, Analytical
Katerina V. Djambazova, Jacqueline M. Van Ardenne, Jeffrey M. Spraggins
Summary: Imaging mass spectrometry allows for the untargeted mapping of biomolecules directly from tissue sections, with widespread clinical applicability in disease diagnosis and classification. This review summarizes the two most widely employed IMS technologies and their advancements in biomedical applications.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Plant Sciences
Yukun Liu, Xiaofei Nie, Jilong Wang, Zhenqi Zhao, Zhimei Wang, Fang Ju
Summary: Flavonoids in litchi seeds have broad-spectrum antiviral and antitumor activities, especially against breast and liver cancers. MALDI-MSI was used to detect and image the distribution of flavonoids in litchi seed tissue sections for the first time, revealing their heterogeneous distribution and potential for extraction.
FRONTIERS IN PLANT SCIENCE
(2023)
Article
Biochemical Research Methods
Cristina Arciniega, Kenneth P. Garrard, Jacob P. Guymon, Jeffrey G. Manni Sr, Alex Apffel, John C. Fjeldsted, David C. Muddiman
Summary: High-throughput screening (HTS) is a technique used by pharmaceutical companies to quickly screen multiple compound libraries for potential drugs. Mass spectrometry (MS) is a popular choice for HTS because it can analyze hundreds to thousands of compounds simultaneously without additional chemical derivatization. In this study, we developed an infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) source coupled directly to an Agilent 6545 mass spectrometer for direct analysis from well plates. The source used a laser operating at 100 Hz with high ionization efficiency, and a metal capillary was constructed to improve ion transmission and sensitivity.
JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Ying Xi, Alexandria L. Sohn, Alena N. Joignant, Stephanie M. Cologna, Boone M. Prentice, David C. Muddiman
Summary: Mass spectrometry imaging (MSI) is an important analytical technique for reporting the spatial location and abundance of detected ions in various studies. However, the lack of consistency in data reporting creates challenges in comparing MSI data. To address this issue, a unified data reporting system called SMART is proposed, which aims to capture essential baseline information for MSI studies. The tutorial emphasizes the necessity of establishing a uniform reporting system to facilitate the interpretation and comparison of MSI data.
JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Seth M. Eisenberg, Kevan T. Knizner, David C. Muddiman
Summary: Mass spectrometry imaging (MSI) is an analytical technique that detects and visualizes thousands of m/z values in two- and three-dimensional space. Discriminating sample-related analytes from ambient ions conventionally requires manual investigation of each ion heatmap, which is time-consuming and subjective. In this study, an ion classification tool (ICT) was developed using object-based image analysis in MATLAB, which accurately classified ions as on-tissue or background based on binary conversion and the number of detected objects.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Correction
Biochemical Research Methods
David C. Muddiman
JOURNAL OF MASS SPECTROMETRY
(2023)
Correction
Biochemical Research Methods
David C. Muddiman
JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Alena N. N. Joignant, Ying Xi, David C. C. Muddiman
Summary: Biospecimens with flat surfaces are needed for laser-based mass spectrometry imaging. However, imperfections in the sampling stages and non-flat samples require a deeper understanding of the laser beam's depth of focus. This tutorial explores the parameters and equations that describe the depth of focus of a Gaussian laser beam and presents methods to address surface roughness exceeding the laser's depth of focus.
JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Russell R. Kibbe, David C. Muddiman
Summary: Profile data collection in mass spectrometry imaging (MSI) studies often results in large files and long processing times. This study compares profile and centroid data collection methods in high-resolution accurate mass MSI. The results show that centroid data collection improves mass measurement accuracy and lipid annotation sensitivity compared to profile data collection.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Mary F. Wang, Alexandria L. Sohn, Juhi Samal, Kevin Erning, Tatiana Segura, David C. Muddiman
Summary: Two preparatory methods for mass spectrometry imaging (MSI), fresh-frozen and sucrose-embedded, paraformaldehyde (PFA) fixed, were evaluated in terms of ion abundance, putative lipid identifications, and preservation of analyte spatial distributions. Sucrose-embedded, PFA-fixed tissues without an ice matrix showed significantly higher numbers of putatively identified lipid species in positive and negative ion modes compared to the traditional gold-standard fresh-frozen tissue preparation with an exogenous ice matrix. Sucrose-embedded tissues also demonstrated improved spatial distribution of ions. These findings support sucrose-embedding without ice matrix as an alternative preparatory technique for IR-MALDESI-MSI.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Tana V. Palomino, David C. Muddiman
Summary: This study presents a new rule that can predict the number of sialic acids on a glycan. By utilizing infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) in negative-ion mode mass spectrometry, the number of sialic acids on the glycan can be predicted based on the experimental isotopic distribution of a detected glycan. This new rule improves the capability of IR-MALDESI to analyze sialylated N-linked glycans within biological tissues, providing confident glycan annotations and compositions.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Ying Xi, Kevan T. T. Knizner, Kenneth P. P. Garrard, David C. C. Muddiman
Summary: This study presents a mass spectrometry imaging (MSI) method that automatically corrects discernible height differences across surfaces during imaging experiments. A chromatic confocal sensor is incorporated into the infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) system to measure the sample surface height at each analytical scan location, allowing for adjustment of the z-axis position of the sample during MSI data acquisition. The method is evaluated using a tilted mouse liver section and an unsectioned Prilosec tablet, showing consistent ablated spot sizes and shapes and revealing the measured ion spatial distribution.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Mary F. Wang, Morgan M. Ritter, Seth W. Kullman, David C. Muddiman
Summary: In this study, the feasibility of sucrose-embedding with paraformaldehyde fixation as an alternative matrix for IR-MALDESI analysis in whole-body zebrafish samples was investigated. The results demonstrated that sucrose-embedding method obtained more lipid annotation information compared to the conventional fresh-frozen sample preparation. This is important for studying and analyzing disease states in whole-body zebrafish.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Juhi Samal, Tana V. Palomino, Judy Chen, David C. Muddiman, Tatiana Segura
Summary: N-linked glycosylation is a complex protein modification that plays a role in cellular signaling and metabolism. Aberrant protein glycosylation is a characteristic feature of many diseases. Spatial profiling of N-glycans through imaging on tissue sections can be used for disease diagnosis. Infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) is a sensitive technique that can be used for mass spectrometry imaging.
ANALYTICAL CHEMISTRY
(2023)
Article
Biochemical Research Methods
Seth M. Eisenberg, Kevan T. Knizner, David C. Muddiman
Summary: Mass spectrometry imaging (MSI) is a technique for measuring and visualizing the spatial distribution of ions in a sample. METASPACE is commonly used for annotation in high-resolution, accurate mass imaging data, but its reported confidence scores often do not accurately reflect the confidence level. The metabolite annotation confidence score (MACS) is an alternative system based on fundamental metrics to generate values that reflect the confidence of an annotation in HRAM-MSI data.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Alena N. Joignant, Morgan M. Ritter, Kevan T. Knizner, Kenneth P. Garrard, Seth W. Kullman, David C. Muddiman
Summary: This study proposes a novel method of mass spectrometry imaging (MSI) to reduce the acquisition time of MSI data using nested regions of interest (nROIs). By utilizing nROIs, a smaller region of interest can be imaged at higher spatial resolution nested within a larger region of interest at lower spatial resolution, conserving maximal spatial and chemical information while decreasing acquisition time. The nROI method was characterized on mouse liver and applied to top-hat MSI of zebrafish, resulting in significant improvements in acquisition time and spatial detail. The nROI method can be applied to any method where acquiring larger high-resolution ROIs poses a practical challenge.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Biochemical Research Methods
Alena N. Joignant, Kevan T. Knizner, Ying Xi, David C. Muddiman
Summary: This study establishes an optimal sample thickness for IR-MALDESI-MSI at around 7 micrometers, as analyzing thicker tissue sections (>10 μm) results in lower ion abundance, decreased signal over long analysis times, and more frequent instrument cleaning.
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
(2023)
