Review
Chemistry, Analytical
Vera Plekhova, Kimberly De Windt, Margot De Spiegeleer, Marilyn De Graeve, Lynn Vanhaecke
Summary: Biofluid metabolomics is a valuable tool for discovering biomarkers related to disease, genetics, and exposure. Direct infusion and ambient ionization mass spectrometry offer attractive alternatives for rapid analysis with minimal sample handling.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
David Moreno-Gonzalez, Delia Castilla-Fernandez, Pascal Vogel, Guanghui Niu, Sebastian Brandt, Carolin Drees, Juan F. Garcia-Reyes, Antonio Molina-Diaz, Joachim Franzke
Summary: This study evaluated the potential of a new plasma-based soft ionization source named CA-F mu TP for the determination of BTEX group in olive oil, showing advantages over EI with easier identification of BTEX mass spectrum. The sensitivity of CA-FmTP was comparable to EI, demonstrating potential usefulness for BTEX analysis in fatty complex matrixes like olive oil.
ANALYTICA CHIMICA ACTA
(2021)
Review
Chemistry, Analytical
Liang Chen, Alireza Ghiasvand, Estrella Sanz Rodriguez, Peter C. Innis, Brett Paull
Summary: Ambient ionization mass spectrometry (AIMS) has developed rapidly in recent years with the introduction of various new ionization techniques, while the application of nanomaterials has also received significant attention, effectively improving selectivity and ionization efficiency.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2021)
Review
Spectroscopy
Hanlu Yue, Feiyao He, Zhongjun Zhao, Yixiang Duan
Summary: Ambient mass spectrometry (AMS) is a group of advanced analytical techniques that enable direct sampling and ionization of analytes in their native environment, offering advantages such as rapid and real-time analysis. Plasma-based AMS, as a significant category of AMS, has been widely applied in various fields and has undergone continuous development and innovation.
MASS SPECTROMETRY REVIEWS
(2023)
Article
Instruments & Instrumentation
George C. -Y. Chan, Carsten Engelhard, Joshua S. Wiley, Ayanna U. Shoulds, R. Graham Cooks, Gary M. Hieftje, Jacob T. Shelley
Summary: In this paper, the optical spectroscopy of the low-temperature plasma (LTP) probe and its interaction with a sample substrate and a grounded metallic needle were investigated. It was found that the LTP probe exhibits important spectral characteristics under certain conditions, which are correlated with the mass-spectral results. Temporally and spatially resolved imaging provided insights into important processes in the LTP plasma jet.
APPLIED SPECTROSCOPY
(2023)
Review
Chemistry, Analytical
Sarmila Amatya Shrestha, Sangwon Cha
Summary: The paper reviews the application of ambient desorption/ionization mass spectrometry in the direct analysis of solid materials, covering various sampling and desorption processes. Real-world analysis cases include pharmaceuticals, food products, forensic analysis, and surface contaminant analysis. ADI techniques provide efficient and simplified methods for direct desorption and ionization of analytes from untreated samples under ambient conditions.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Analytical
Lucia Bartella, Marcos Bouza, Priscilla Rocio-Bautista, Leonardo Di Donna, Juan F. Garcia-Reyes, Antonio Molina-Diaz
Summary: Ambient mass spectrometry is an alternative to classical mass spectrometry that allows fast, in-situ, and high-throughput analysis of samples with minimal sample pretreatment. This study explores the capability of different ambient ionization sources to analyze raw wine for quality control purposes. The spectra obtained from these sources showed the ability to classify and differentiate wine samples based on various compounds, including organic acids, phenolic acids, derivatives, and low-molecular-mass flavonoids. The plasma-based methods offer the advantage of solventless analysis, while the paper spray (PS) approach provides a richer MS profile.
MICROCHEMICAL JOURNAL
(2022)
Article
Chemistry, Analytical
Maryam Aghaei, Annemie Bogaerts
Summary: In this study, plasma chemistry in a helium flowing atmospheric pressure afterglow (FAPA) for analytical spectrometry is described using a quasi-one-dimensional plasma chemical kinetics model. The model demonstrates the formation of H, N, and O atoms in the discharge region, and the dominance of O-3 and NO species in the afterglow. Helium plays a key role in Penning ionization and charge transfer reactions, leading to high analytical sensitivity. The model's predictions align with previous observations in the literature, providing insights to enhance analytical performance of ambient desorption/ionization sources.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Analytical
Vincen Wu, Jocelyn Tillner, Emrys Jones, James S. McKenzie, Dipa Gurung, Anna Mroz, Liam Poynter, Daniel Simon, Cristina Grau, Xavier Altafaj, Marc-Emmanuel Dumas, Ian Gilmore, Josephine Bunch, Zoltan Takats
Summary: This study examines the suitability of desorption electro-flow focusing ionization (DEFFI) for mass spectrometry imaging (MSI) of biological tissue, comparing its performance to the traditional desorption electrospray ionization (DESI). The flow focusing mechanism in DESI offers advantages such as a rotationally symmetric electrospray jet, higher intensity, controllable parameters, and better portability. The optimized parameters for DEFFI result in similar images to DESI but with better sensitivity.
ANALYTICAL CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Hung Su, Zong-Han Jiang, Shu-Fen Chiou, Jentaie Shiea, Deng-Chyang Wu, Sung-Pin Tseng, Shu-Huei Jain, Chung-Yu Chang, Po-Liang Lu
Summary: An analytical platform combining probe sampling, thermal desorption-electrospray ionization/mass spectrometry (TD-ESI/MS), and multivariate statistical analysis was developed to rapidly differentiate bacterial species based on the differences in their lipid profiles. The results were validated by protein fingerprinting using matrix-assisted laser desorption ionization time-of-flight (MALDI-TOF). The developed platform showed promising potential as a useful diagnostic tool for rapidly distinguishing bacterial species.
Article
Chemistry, Analytical
Xiaoping Zhang, Xiang Ren, Yuan Zhong, Konstantin Chingin, Huanwen Chen
Summary: The study detected ketones in exhaled breath using mass spectrometry and developed a fast, sensitive, noninvasive method for ketone analysis. Results showed higher levels of acetone in the breath of smokers compared to non-smokers.
Article
Biochemical Research Methods
Luan Felipe Campos Oliveira, Damila Rodrigues de Morais, Deleon Nascimento Correa, Jacqueline de Morais Campelo, Alessandra Sussulini, Marcos Nogueira Eberlin, Jandyson Machado Santos
Summary: The study proposed a method to identify artificially aged papers using EASI-MS analysis, successfully identifying the most relevant ions through multivariate statistical analysis and HRMS technology, which can help identify chemical additives in counterfeit documents and be used in forensic laboratories.
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
(2021)
Article
Multidisciplinary Sciences
Margot De Spiegeleer, Vera Plekhova, Jozefien Geltmeyer, Ella Schoolaert, Beata Pomian, Varoon Singh, Kathleen Wijnant, Kimberly De Windt, Volter Paukku, Alexander De Loof, Inge Gies, Nathalie Michels, Stefaan De Henauw, Marilyn De Graeve, Karen De Clerck, Lynn Vanhaecke
Summary: In recent years, ambient ionization mass spectrometry (AIMS) has allowed for direct analysis of biofluid metabolome. However, AIMS procedures are hindered by analytical and practical limitations, which affect metabolome coverage. This study aimed to develop biofluid-specific metabolome sampling membranes (MetaSAMPs) to improve AIMS. Customized MetaSAMPs made of hydrophilic and lipophilic polymers demonstrated superior metabolome coverage and transport stability compared to crude biofluid analysis. This new approach was successfully validated and has potential applications in metabolic health stratification.
Article
Chemistry, Analytical
Carmina Vejar-Vivar, Jaime Millan-Santiago, Claudia Mardones, Rafael Lucena, Soledad Cardenas
Summary: This study evaluates polydopamine inner wall-coated hypodermic needles as microextraction devices and electrospray ionization emitters for determining illicit drugs in oral fluid samples.
Article
Biochemical Research Methods
Christopher C. Goudarzi, Ashley G. Woolfork, Arjun Sengupta, Aalim M. Weljie
Summary: Increased access to cheap and rapid mass spectrometry testing of biofluids is desired for the analysis of disorders and diseases related to metabolite or lipid level changes. This study establishes a customized high-throughput workflow for biological sample analysis using DESI-MS, which utilizes low-cost, open-source, and readily accessible materials. The workflow includes surface customization, high-throughput sample spotting, and an open-source interface for data analysis. The developed system allows for cost-effective custom surface design workflows and high-throughput analyses for a wide range of researchers.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Chemistry, Analytical
Lucas J. Szalwinski, L. Edwin Gonzalez, Nicolas M. Morato, Brett M. Marsh, R. Graham Cooks
Summary: In this study, the growth of E. coli was monitored using desorption electrospray ionization mass spectrometry, and changes in lipids were observed. The study also demonstrated the potential of desorption electrospray ionization mass spectrometry for rapid sampling of complex mixtures.
Article
Chemistry, Medicinal
Samadhi C. Kulathunga, Nicolas M. Morato, Qing Zhou, R. Graham Cooks, Andrew D. Mesecar
Summary: A novel label-free assay based on high-throughput DESI-MS and a fluorometric coupled-enzyme method were developed for quantitation and kinetic analysis of the sulfonation reaction catalyzed by SULT2B1b. Both methods provided consistent kinetic data and indicated the affinity trend of SULT2B1b with its substrates. The DESI-MS assay has promising potential for identifying SULT2B1b inhibitors as prostate cancer therapeutics and can be applied to other drug discovery efforts.
Article
Chemistry, Analytical
Marcos Bouza, Julio Garcia-Martinez, Bienvenida Gilbert-Lopez, Sebastian Brandt, Juan F. Garcia-Reyes, Antonio Molina-Diaz, Joachim Franzke
Summary: Dielectric barrier discharge ionization (DBDI) is a versatile tool for small-molecule mass spectrometry applications, covering a wide range of molecules from polar to low polar. However, the complex plasma gas-phase interactions in DBDI have not been well studied. In this study, the ionization mechanisms of a two-ring DBDI ion source were evaluated using different discharge gases for vaporized liquid samples. The results showed that APCI and DBDI exhibited different ionization trends during PAH analysis, with APCI mainly producing [M + H]+ ions and DBDI showing the prevalence of charge exchange reactions. The addition of dopants in the gas phase shifted the ionization mechanisms towards charge exchange reactions and facilitated the formation of [M]??+ ion species.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Applied
Atalanti Christou, Ana B. Martinez-Piernas, Ioannis J. Stavrou, Juan F. Garcia-Reyes, Constantina P. Kapnissi-Christodoulou
Summary: The effects of ripening stage, processing method, and geographical origin on the chemical composition and properties of Carob were investigated in this study using HPLC-ESI-HRMS and chemometric analysis. The study found that Carob seeds had higher levels of polyphenols, and unripe pods were richer in polyphenols. Carob processing, particularly thermal treatment, also led to noticeable changes in its chemical composition. The geographical origin also had an impact on the phenolic composition of Carob.
JOURNAL OF FOOD COMPOSITION AND ANALYSIS
(2022)
Review
Chemistry, Analytical
Priscilla Rocio-Bautista, David Moreno-Gonzalez, Ana B. Martinez-Piernas, Juan F. Garcia-Reyes, Antonio Molina-Diaz
Summary: This review discusses the application of liquid chromatography-mass spectrometry (LC-MS) technique in the determination of glyphosate (Gly) and related compounds. The sample preparation methods and novel liquid chromatography/mass spectrometry approaches are introduced, and the analytical challenges, strengths, and drawbacks are critically discussed.
TRENDS IN ENVIRONMENTAL ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Kai-Hung Huang, Nicolas M. Morato, Yunfei Feng, R. Graham Cooks
Summary: Late-stage diversification of drug molecules is facilitated by reaction screening using high-throughput experimentation. In this study, a rapid method for functionalizing bioactive molecules based on accelerated reactions in microdroplets is presented. Using this method, an opioid agonist and an antagonist were diversified and characterized by tandem mass spectrometry after screening over 500 reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Physics, Atomic, Molecular & Chemical
Eric T. Dziekonski, Thomas C. Sams, Lucas J. Szalwinski, L. Edwin Gonzalez, R. Graham Cooks
Summary: Two-dimensional tandem mass spectrometry (2D-MS/MS) is employed to characterize each sample in an array by creating ion populations from complex mixtures using desorption electrospray ionization. Automated high-throughput examination of each sample in the array is achieved through integrated movement of the sample array and automated data acquisition. Position control is accomplished using an Arduino microprocessor, a RAMPS control board, two stepper motors, and a custom MATLAB graphical user interface. Data processing improvements are made to enhance visual discrimination of peaks from the background in local regions of the 2D spectrum.
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Chemistry, Multidisciplinary
R. Graham Cooks, Yunfei Feng, Kai-Hung Huang, Nicolas M. Morato, Lingqi Qiu
Summary: The article argues that mass spectrometry (MS) can be used sequentially for the three key steps in drug discovery: reaction screening, synthesis scale-up, and bioactivity assessment. The chosen ionization method, desorption electrospray ionization (DESI), is both an analytical technique and a procedure for small-scale synthesis. DESI is highly compatible with automation, allowing for high throughput in both synthesis and analysis.
ISRAEL JOURNAL OF CHEMISTRY
(2023)
Review
Chemistry, Analytical
Jyotirmoy Ghosh, R. Graham Cooks
Summary: Mass spectrometry (MS), a century-old analytical technique, is now being used as a preparative method. Electrospray deposition (ESD) of charged droplets generated by electrospray ionization (ESI) is an efficient way to form nanomaterials, including catalysts. By using mass-analyzed ions and performing ion soft landing (SL), higher chemical specificity in surface modification can be achieved, although this vacuum-based method is slow due to low ion currents. MS-based synthesis by ESD or SL provides advantages over traditional approaches, allowing control over material properties and surface patterning without the need for additives or reducing agents.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Nicolas M. Morato, R. Graham Cooks
Summary: Mass spectrometry (MS) is widely used in the chemical sciences for various applications such as monitoring reaction products, identifying disease biomarkers, and measuring thermodynamic parameters. Electrospray ionization (ESI) is a commonly used method to ionize polar compounds from solution. Desorption electrospray ionization (DESI) is a technique that directly generates ions from objects in the ambient environment. The simplicity and wide applicability of DESI revolutionized the analysis of complex materials for their organic components, particularly for in situ applications.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Analytical
Marcos Bouza, Norman Ahlmann, Juan F. Garcia-Reyes, Joachim Franzke
Summary: The present study investigated the potential of SALD-FμTP-MS as a rapid analytical technique for direct analysis of surface-deposited samples. Paper was used as the substrate and an infrared hand-held laser was employed for sample desorption. The optimization process involved the use of viscous solvents to enhance desorption and ionization efficiencies. Ethylene glycol (EG) was identified as a suitable solvent, improving sensitivity and substrate stability. The applicability of SALD-FμTP-MS was demonstrated by successfully analyzing food, water, and biological samples, particularly for thermolabile and polarity diverse compounds.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Lingqi Qiu, Mousumi Saha, Stefan Kraft, Eric T. Dziekonski, Christopher J. Welch, Yumin Dai, Andreas Kaerner, R. Graham Cooks
Summary: This study employs a rapid tandem mass-spectrometry method for determining water content in complex organic solutions, with a focus on trace-water analysis. Water is captured using a charge-labeled molecular probe, which selectively binds to the strongly electrophilic aldehyde site. This method allows for quantitative determinations over a wide concentration range with high accuracy and short analysis times.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Physics, Atomic, Molecular & Chemical
Eric T. Dziekonski, Gregory S. Eakins, R. Graham Cooks
Summary: In this study, an Arduino Uno microcontroller is used to control several electrical/electromechanical switches and the timing of all experimental subsystems in response to the instrument trigger output and a user selected operating mode. By calibrating and measuring the RF amplitude control signal in 1D mode, it is possible to calculate the applied RF amplitude in 2D mode, thereby allowing the user to determine relevant quadrupole operating parameters for a particular sample.
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
(2023)
Article
Chemistry, Analytical
Andres J. Rascon, Priscilla Rocio-Bautista, David Moreno-Gonzalez, Juan F. Garcia-Reyes, Evaristo Ballesteros
Summary: The metal-organic framework CIM-80(Al) was proposed as a sorbent coating for solid-phase microextraction fibers. The CIM-80(Al)-based microextraction fibers with a thickness of 3.5 μm were used to isolate and determine 14 phthalate esters in bottled water with promising results. The extraction efficiency was comparable to commercial coatings in a total of 16 bottled water samples.
MICROCHEMICAL JOURNAL
(2023)
Article
Chemistry, Analytical
Sangeeta Pandey, Yanyang Hu, Peter L. Anderson, Jennifer J. Kiser, R. Graham Cooks
Summary: We validate the concept of point-of-care assessment of long-term alcohol consumption by measuring phosphatidylethanol in blood/dried blood spots using nano-electrospray ionization and MS/MS with a miniature mass spectrometer. The levels of "abstinence", "moderate", and "chronic" consumption can be rapidly distinguished for both sample types, and quantitative analysis is achieved with blood samples (LoQ-100 ng mL(-1)).
