Review
Chemistry, Analytical
Katie M. Kohoutek, Peter de B. Harrington
Summary: Electrospray ionization ion mobility mass spectrometry (ESI-IMS-MS) is a rapidly progressing analytical technique that examines complex compounds in the gas phase. It separates isomers, provides structural information, and quantitatively identifies various compounds in biological samples. ESI-IMS-MS has wide applications in pharmaceutical, environmental, and manufacturing industries.
CRITICAL REVIEWS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
A. Bianco, I Neefjes, D. Alfaouri, H. Vehkamaki, T. Kurten, L. Ahonen, M. Passananti, J. Kangasluoma
Summary: Mass spectrometry is an effective method for identifying and quantifying environmentally relevant molecules, but it cannot distinguish between isomers. This study combines an experimental set-up using a differential mobility analyser with computational ion mobility calculations to successfully identify isomers. The experimental set-up allows for analysis in both the gas and liquid phase, making it a versatile tool for isomer separation.
Article
Chemistry, Analytical
Wen Liu, Yanjing Chen, Fei Liu, Xurong Yin, Jiayi Cai, Yong Xia, Jianna Yu, Guoxing Jing, Wenshan Li, Wenjie Liu
Summary: A method using electrospray ionization-ion mobility spectrometry (ESI-IMS) combined with a metal ion-assisted technique was developed for rapid and simultaneous determination of carbendazim and thiabendazole residues. The Cu(II) assisted approach helped to achieve well-separated peaks. The method showed good performance in the detection of both carbendazim and thiabendazole in different fruits.
Article
Chemistry, Multidisciplinary
Nina Khristenko, Frederic Rosu, Eric Largy, Jerome Haustant, Cedric Mesmin, Valerie Gabelica
Summary: Native ion mobility mass spectrometry has potential applications in the biophysical characterization of proteins, as the charge state distribution and collision cross section distribution depend on the solution conformation. This study investigates the charging and gas-phase conformation of multi-domain therapeutic proteins with globular domains tethered by disordered linkers. The results suggest a hybrid ionization mechanism, where globular domains are ejected one at a time from a parent droplet.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Biochemical Research Methods
Rebecca L. Cain, Ian K. Webb
Summary: Electrospray ionization mass spectrometry (ESI-MS) experiments were used to study the solution-like structures of intact proteins, specifically by controlling the protein unfolding process and analyzing folding intermediates. By mixing various pH solutions online with aqueous cytochrome C, the changes in charge states, arrival time distributions (ATDs), and electron capture dissociation (ECD) were measured to detect folding intermediates and unfolded protein structures.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Article
Biochemical Research Methods
J. Michael Sutton, Noha M. El Zahar, Michael G. Bartlett
Summary: The study focuses on improving the mobile phase of electrospray oligonucleotides to reduce spectral complexity and increase sensitivity. By using different combinations of fluorinated alcohols and alkylamines, it is possible to selectively reduce the charge states of oligonucleotides. Additionally, anionic salts are used to stabilize complexes and provide unique structural information about the molecules.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Review
Biochemistry & Molecular Biology
Luisa-Gabriela Bogos, Ioana-Ecaterina Pralea, Radu-Cristian Moldovan, Cristina-Adela Iuga
Summary: Chiral metabolomics is a fast-growing research field, driven by recent advances in separation techniques. This review summarizes the most significant developments in indirect enantioseparations of endogenous metabolites over the past 10 years, including improvements in chiral derivatizing agents and new separation methodologies. It also highlights exciting advancements in separation techniques combined with mass spectrometry, which offer new possibilities for characterizing chiral metabolites in complex samples and improve understanding of their roles in systems biology.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Biochemical Research Methods
Frederik Lermyte, Alina Theisen, Peter B. O'Connor
Summary: Biomolecular ions in mass spectrometry are characterized by their net charge, with methods existing to manipulate this quantity in the gas phase. The charge site of ions can significantly affect their gas-phase behavior, and research on this is particularly lacking for peptides and intact proteins. A study identified two distinct protonation site isomers of α-synuclein at the same charge state, showing differences in gas-phase fragmentation behavior and distinguishable by ion mobility spectrometry. Charge sites for both protomers were determined using ultraviolet photodissociation.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Chemistry, Analytical
Fuxing Xu, Shutong Yang, Fangling Wu, Chuan-Fan Ding
Summary: In this study, a rapid and simple method for the isomeric recognition of dipeptides was developed using electrospray ionization (ESI) and trapped ion-mobility mass spectrometry (TIMS-MS). The chiral structure of different dipeptides could be distinguished by beta-CD, and the relative content of isomeric dipeptides mixtures was measured. This method provides a direct analytical tool for determining isomeric dipeptides and has potential applications in chiral recognition.
MICROCHEMICAL JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Yao Qian, Xiangyu Guo, Yunfang Wang, Zheng Ouyang, Xiaoxiao Ma
Summary: A mobility-modulated sequential dissociation (MMSD) strategy was developed for mass spectrometry imaging, enabling spatial lipidomics capable of multiplexed MS/MS imaging of 24 structurally distinct lipids. The method revealed a potential biomarker in a human hepatocellular carcinoma tissue.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Analytical
Daniel G. Delafield, Gaoyuan Lu, Cameron J. Kaminsky, Lingjun Li
Summary: Mass spectrometry-based biomolecular analyses have become popular in research settings. Gas phase ion separation techniques provide a fourth dimension of analysis, enabling rapid characterization and high throughput profiling. This review highlights the latest developments and applications of high-end ion-mobility enabled instruments and their advantages for biomolecular research.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Applied
Minna Juvonen, Edwin Bakx, Henk Schols, Maija Tenkanen
Summary: This study investigated the potential of using TWIMS and CID-TWIMS-MS/MS to separate cereal-derived isomeric arabinoxylanoligosaccharides (A)XOS. The triand pentasaccharide isomers were distinguishable by the ATDs of the precursor ions, while CID-TWIMS-MS/MS could effectively separate isomeric fragment ions produced from tetra- and pentasaccharide (A)XOS. The base peak mobility spectrum was also introduced as a practical tool for (A)XOS fingerprinting.
Article
Chemistry, Multidisciplinary
Karen E. Butler, Yoshihiko Takinami, Adam Rainczuk, Erin S. Baker, Blaine R. Roberts
Summary: Native mass spectrometry combined with IMS-MS technology can be used to study the tertiary and quaternary structure of proteins, validate other structural determination methods, and provide more comprehensive structural information.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Ondrej Jurcek, Nonappa, Elina Kalenius, Pia Jurcek, Juha M. Linnanto, Rakesh Puttreddy, Hennie Valkenier, Nikolay Houbenov, Michal Babiak, Miroslav Peterek, Anthony P. Davis, Radek Marek, Kari Rissanen
Summary: Constructing structurally complex architectures using unique ligands is a challenge in metallosupramolecular chemistry, but a superchiral Pd3L6 complex can be obtained via supramolecular transmetalation reactions. These complexes can self-organize into hexagonal microparticles in aqueous media, potentially leading to the development of novel metal-organic functional materials made of natural, abundant, and relatively inexpensive steroidal compounds.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Jan Leipert, Philipp T. Kaulich, Max K. Steinbach, Britta Steer, Konrad Winkels, Christine Blurton, Matthias Leippe, Andreas Tholey
Summary: Researchers have developed a sample preparation method based on protein aggregation and acidic elution, allowing for sensitive protein identification analysis of single nematodes on a digital microfluidics device. Compared to in-tube sample preparation, this method increases proteoform identifications by 46%. Label-free quantification also reveals changes in proteoform abundance that cannot be distinguished by bottom-up proteomics. This workflow facilitates proteoform-focused analysis on limited availability samples.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Lauryn E. DeGreeff, Alison G. Simon, Michael S. Macias, Howard K. Holness, Kenneth G. Furton
Summary: COMPS is a controlled odor release system that provides instant and reproducible source of odorant vapor by sealing odorants in permeable bags. This system is used for olfactory testing and training, with the ability to adjust the release rate and concentration of odorants.
JOVE-JOURNAL OF VISUALIZED EXPERIMENTS
(2021)
Article
Chemistry, Analytical
Stephanie R. Vaughan, Lauryn E. DeGreeff, Leann Forte, Howard K. Holness, Kenneth G. Furton
Summary: The powerful nature of fentanyl presents significant dangers to both abusers and law enforcement personnel, emphasizing the need for a non-contact detection method. The exploration of fentanyl's volatile signature using SPME-GC-MS provides a crucial foundation for the future development of a non-contact vapor detection method for fentanyl.
FORENSIC CHEMISTRY
(2021)
Article
Automation & Control Systems
Daniel Ramos, Juan Maronas, Jose Almirall
Summary: The calibration of likelihood ratios generated using previous models is crucial for realistic reporting of glass evidence comparisons. Our proposed models, which incorporate heavy-tailed within-source variability and probabilistic machine learning algorithms for between-source variability, outperform previous LR models and show superior performance in calibration and robustness.
CHEMOMETRICS AND INTELLIGENT LABORATORY SYSTEMS
(2021)
Article
Medicine, Legal
Vidia A. Gokool, Howard K. Holness, Kenneth G. Furton
Summary: This study investigates the variation in human hand odor samples over time and the accuracy in associating these samples. The results show that there is greater variation among samples from different days and different subjects, while less variation is observed among samples from the same subject on different days. Two proof of concept models for determining sample source origin were developed with high performance measures.
FORENSIC SCIENCE INTERNATIONAL
(2022)
Article
Chemistry, Analytical
Alexander Acosta, Jose Almirall
Summary: The Fast Blue BB colorimetric test effectively distinguishes between different cannabinoids in cannabis, particularly THC, demonstrating selectivity for THC while differentiating between hemp and marijuana. The test successfully classified samples with THC levels below 0.3% (hemp) and those with higher THC levels and lower CBD levels (marijuana), but struggled with samples containing slightly above 0.3% THC and high CBD content. Additionally, herbs and spices were accurately distinguished from cannabis samples in the test.
FORENSIC CHEMISTRY
(2021)
Article
Chemistry, Analytical
Jacqueline L. Rodriguez, Jose R. Almirall
Summary: The study utilized a dynamic sampling and preconcentration device, CMV, coupled with a portable GC-MS for rapid detection of volatile organic compounds associated with explosives. Different sampling methods achieved sub-nanogram instrumental detection limits for various analytes of interest. A novel continuous vapor delivery system improved analyte recovery rates significantly in a shorter sampling time.
FORENSIC CHEMISTRY
(2021)
Article
Chemistry, Analytical
Anuradha Akmeemana, Ruthmara Corzo, Jose Almirall
Summary: This paper introduces a new R-based Shiny GUI for calculating calibrated likelihood ratios (LRs) using three different background databases of glass composition, providing valuable insights into forensic glass analysis. The study demonstrates how LLR values increase with the size of the background database, highlighting the effectiveness of the method in forensic investigations. The R Shiny app and the newly introduced FIU vehicle background database are valuable resources for researchers in the field.
FORENSIC CHEMISTRY
(2022)
Article
Chemistry, Analytical
Katelyn Lambert, Shirly Montero, Anuradha Akmeemana, Ruthmara Corzo, Gwyneth Gordon, Emily Haase, Ping Jiang, Oriana Ovide, Katrin Prasch, Kahlee Redman, Thomas Scholz, Tatiana Trejos, Jodi Webb, Peter Weis, Wim Wiarda, Sharon Wilczek, Huifang Xie, Peter Zoon, Jose Almirall
Summary: Ten different laboratories conducted an interlaboratory study using LA-ICP-MS and ASTM E2927 method for the analysis and comparison of glass evidence. The study aimed to evaluate the performance of a new calibration standard, comparison criteria, and the use of LR for quantitative determination of evidence strength. Results showed distinguishability between glass from the same windowpane and different vehicles based on LR values.
FORENSIC CHEMISTRY
(2022)
Article
Chemistry, Analytical
Michelle N. Torres, Jose R. Almirall
Summary: The novel dynamic headspace extraction device, CMV, when coupled with a person-portable GC-MS, demonstrated effectiveness for the analysis of ILRs in field sampling. The use of a paper cup in conjunction with CMV for in-field VOC sampling was introduced for the first time. CMV showed greater extraction capabilities than portable GC-MS and higher sensitivity compared to traditional extraction techniques.
FORENSIC CHEMISTRY
(2022)
Article
Chemistry, Analytical
Claudia Martinez-Lopez, Oriana Ovide, Ruthmara Corzo, Zachary Andrews, Jose R. Almirall, Tatiana Trejos
Summary: This study evaluates the capability of mu-XRF and LIBS analyses compared to LA-ICP-MS for characterizing glass homogeneity. The results show that error rates below 3% can be achieved for mu-XRF and LIBS when selecting the appropriate number of fragments, measurements, and comparison criterion.
FORENSIC CHEMISTRY
(2022)
Article
Chemistry, Analytical
Kimiko Ferguson, Sherri L. Tupik, Hunter Haddad, Jeannette Perr, Michael Gilbert, Reta Newman, Jose Almirall
Summary: Forensic laboratories use both gas chromatography mass spectrometry (GC-MS) and gas chromatography Fourier-transform infrared spectroscopy (GC-IR) for the identification of controlled substances. A novel fentanyl library consisting of 212 different fentanyl related substances (FRS) reference compounds was created, which can be used for future research and identification purposes.
FORENSIC CHEMISTRY
(2022)
Article
Medicine, Legal
Nicole B. Valdes, Jose R. Almirall
Summary: A new headspace sampling method using the CMV device was demonstrated for the analysis of ILRs in fire debris, achieving fast and ultra-sensitive results. The method involves the use of a heated can for the recovery of VOCs from petroleum distillates. The heated can method showed improved mass recovery and decreased variability compared to the non-heated paper cup method.
JOURNAL OF FORENSIC SCIENCES
(2023)
Article
Chemistry, Analytical
Vidia A. Gokool, Janet Crespo-Cajigas, Amritha Mallikarjun, Amanda Collins, Sarah A. Kane, Victoria Plymouth, Elizabeth Nguyen, Benjamin S. Abella, Howard K. Holness, Kenneth G. Furton, Alan T. Charlie Johnson, Cynthia M. Otto
Summary: In this study, the performance of trained detection dogs and a noninvasive analytical instrumentation method were compared in identifying COVID-19 positive individuals. The results showed that dogs performed better than the computational model when faced with non-ideal samples.
Article
Medicine, General & Internal
Janet Crespo-Cajigas, Vidia A. A. Gokool, Andrea Ramirez Torres, Liam Forsythe, Benjamin S. S. Abella, Howard K. K. Holness, Alan T. Charlie Johnson, Richard Postrel, Kenneth G. G. Furton
Summary: Since the outbreak of the COVID-19 pandemic, there has been significant interest in developing rapid detection measures. This study explored the use of hand odor samples and analytical instrumentation to detect SARS-CoV-2-infected individuals. By analyzing volatile organic compounds (VOCs) extracted from hand odor samples, predictive models were developed using sparse partial least squares discriminant analysis. The research highlights the potential of using odor signatures as a diagnostic tool and lays the foundation for optimizing other rapid screening sensors.
Article
Multidisciplinary Sciences
Chantrell J. G. Frazier, Vidia A. Gokool, Howard K. Holness, DeEtta K. Mills, Kenneth G. Furton
Summary: This study used HS-SPME-GC-MS to analyze human hand odor samples and found that PLS-DA, OPLS-DA, and LDA models can effectively classify and predict gender based on the VOC signatures. The results provide a working model for predicting donor class characteristics using human hand odor profiles.