Article
Chemistry, Multidisciplinary
Xiaowei Song, Qingce Zang, Chao Li, Tianhao Zhou, Richard N. N. Zare
Summary: We developed an immunoassay-based desorption electrospray ionization mass spectrometry imaging (immuno-DESI-MSI) technique for visualizing functional macromolecules. Boronic acid mass tags (BMTs) were synthesized to label antibodies as MSI probes, which can be released from the antibody by cleaving the boronic ester bond under acidic conditions. The BMTs can work in both optical and MS imaging modes and can be readily identified due to the introduction of the boron element.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
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)
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)
Review
Pharmacology & Pharmacy
Manman Qin, Yuqing Qian, Lu Huang, Chao Zhong, Mingdong Li, Jun Yu, Huanwen Chen
Summary: Extraction electrospray ionization mass spectrometry (EESI-MS) enables effective ionization of trace molecules in complex samples without sample pretreatment, providing high sensitivity, selectivity, and response speed. It also allows for advanced functionalization of high-energy molecular species. This article systematically reviews the effects of operating conditions on the analytical performance of EESI-MS for various pharmaceutical compounds and introduces its potential application in molecular functionalization for drug discovery.
FRONTIERS IN PHARMACOLOGY
(2023)
Article
Biochemistry & Molecular Biology
Margaux Fresnais, Siwen Liang, Deniz Seven, Nevena Prodanovic, Julia Sundheimer, Walter E. Haefeli, Juergen Burhenne, Remi Longuespee
Summary: The development and validation of desorption/ionization mass spectrometric assays for drug quantification in tissue sections is crucial for their widespread application in (clinical) pharmacology. Advances in desorption electrospray ionization have demonstrated its usefulness for developing targeted quantification methods that meet validation requirements. Factors such as desorption spot morphology, analytical time, and sample surface need to be considered for successful method development. This study highlights the importance of considering desorption kinetics during DESI analyses, which can help reduce analytical time, verify solvent-based drug extraction methods, and predict feasibility of imaging assays. These findings provide valuable guidance for future development of validated DESI-profiling and imaging methods.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Materials Science, Multidisciplinary
Jean-Arthur Amalian, Tathagata Mondal, Evgeniia Konishcheva, Gianni Cavallo, Benoit Eric Petit, Jean-Francois Lutz, Laurence Charles
Summary: Sequence-defined synthetic polymers are being used as a medium to store information at the molecular level, with low storage capacity of readable chains being a current limitation. Ordering short oligomers on surfaces to compose long messages is an attractive alternative, and desorption electrospray ionization (DESI) is shown to be suitable for bidimensional data storage.
ADVANCED MATERIALS TECHNOLOGIES
(2021)
Article
Biochemistry & Molecular Biology
Sangwon Cha, Gyouwoong Jun, Yougyeong Park, Sung Jun An, Donghoon Lee
Summary: Nanospray desorption electrospray ionization (nano-DESI) was used to analyze the metabolite fingerprints on Hypericum leaves. The intensity changes of key metabolites over time were observed through full mass scan experiments and monitored using selected ion monitoring and pseudo-selected reaction monitoring experiments. The correlation between the time-dependent changes in the metabolite fingerprints and depth-wise metabolite distribution was examined by removing the surface layers of the leaves multiple times.
Article
Chemistry, Analytical
Fengjian Chu, Gaosheng Zhao, Wangyu Li, Wei Wei, Weiwei Chen, Zihan Ma, Zhan Gao, Nazifi Sani Shuaibu, Jikui Luo, Bingwen Yu, Hongru Feng, Yuanjiang Pan, Xiaozhi Wang
Summary: A microwave plasma torch-based ion/molecular reactor (MPTIR) has been developed for creating and monitoring rapid oxidation reactions without the addition of external oxidants or catalysts. The oxidation products from the MPTIR match those of the long-term environmental oxidative process, and two unreported environmental compounds were identified in actual water samples using this device.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Medicinal
Margaux Fresnais, Siwen Liang, Marius Breitkopf, Joshua Raoul Lindner, Emmanuelle Claude, Steven Pringle, Pavel A. Levkin, Konstantin Demir, Julia Benzel, Julia Sundheimer, Britta Statz, Kristian W. Pajtler, Stefan M. Pfister, Walter E. Haefeli, Juergen Burhenne, Remi Longuespee
Summary: Desorption/ionization-mass spectrometric methods are advantageous for the analysis of solid biological matrices. The development of drug quantification assays using DESI has been challenging, but new prototype source setups show promise for targeted quantitative analyses.
Article
Chemistry, Analytical
Xian-Na Wang, Bin Li
Summary: Gold nanoparticles/thiol-beta-cyclodextrin-functionalized TiO2 nanowires were prepared to enhance the performance of SALDI MS and MSI, showing superior detection sensitivity and repeatability.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Analytical
Xufang Hu, Zongping Wang, Haolin Chen, An Zhao, Nianrong Sun, Chunhui Deng
Summary: An advanced metabolic analysis tool based on highly porous metal oxides derived from metal-organic frameworks (MOFs) is developed in this study. The tool successfully differentiates and stages renal cell carcinoma (RCC), as well as identifies the size of tumors. This achievement shows promising prospects for designer matrix-based analytical tools in disease diagnosis.
ANALYTICAL CHEMISTRY
(2022)
Review
Chemistry, Analytical
Bin Hu, Zhong-Ping Yao
Summary: This article reviews the technical aspects and important applications of wooden-tip ESI-MS in various fields. Wooden-tip ESI-MS has shown significant achievements in the past 10 years and has the potential for further development and application.
ANALYTICA CHIMICA ACTA
(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
Biochemical Research Methods
Meiling Huo, Zhonghua Wang, Wenqing Fu, Lu Tian, Wanfang Li, Zhi Zhou, Yanhua Chen, Jinfeng Wei, Zeper Abliz
Summary: Spatially resolved metabolomic method utilizing AFADESI-MSI was used to study region-specific metabolic disturbances in the brains of diabetic rats. 19 discriminating metabolites related to various metabolic pathways were identified and located in the brains of the diabetic rats for the first time, providing valuable insights into the molecular pathological signature of diabetic encephalopathy.
JOURNAL OF PROTEOME RESEARCH
(2021)
Article
Biochemical Research Methods
Consuelo J. Perez, Demian R. Ifa
Summary: A model case study was developed to evaluate three internal standard (IS) application strategies in the DESI-MSI analysis of psycholeptic phenobarbital and isotopically labelled IS phenobarbital-D5 from in vitro dosed tissues of the golden apple snail. Methods I and II showed similar performance in terms of precision and accuracy, while method III requires further research for future quantitative DESI-MSI analyses.
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
(2021)
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, Multidisciplinary
Kai-Hung Huang, Jyotirmoy Ghosh, Shiqing Xu, R. Graham Cooks
Summary: Late-stage functionalization is an approach to generate modified molecules that retain functional groups present in the active drugs. This study characterizes the potential value of high-throughput desorption electrospray ionization mass spectrometry (HT DESI-MS) for small-scale rapid late-stage functionalization.
Article
Chemistry, Multidisciplinary
Xingshuo Chen, Zhenwei Wei, Kai-Hung Huang, Mycah Uehling, Michael Wleklinski, Shane Krska, Alexey A. Makarov, Timothy Nowak, R. Graham Cooks
Summary: In this study, nanoelectrospray ionization mass spectrometry (nanoESI-MS) was used to monitor the precatalysts, catalytic intermediates, reagents, and products of the Suzuki-Miyaura cross-coupling reaction. Pd cluster ions related to the active catalyst and an oxidized catalyst were detected, with the latter increasing as the reaction proceeds. Further experiments confirmed the presence of the oxidized catalyst. Monitoring the formation and conversion of the oxidative addition intermediate provided insights into the progress of the transmetalation step in the catalytic cycle.
Article
Biochemical Research Methods
Lingqi Qiu, Michael D. Psimos, R. Graham Cooks
Summary: This study reports the accelerated oxidation of aromatic sulfones in microdroplets, which shows a high reaction rate and regioselectivity. Experimental data suggest that the water radical cation derived from traces of water in the solvent acts as the oxidant.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Oncology
Manu Prasad, Jonathan Zorea, Sankar Jagadeeshan, Avital B. Shnerb, Sooraj Mathukkada, Jebrane Bouaoud, Lucas Michon, Ofra Novoplansky, Mai Badarni, Limor Cohen, Ksenia M. Yegodayev, Sapir Tzadok, Barak Rotblat, Libor Brezina, Andreas Mock, Andy Karabajakian, Jerome Fayette, Idan Cohen, Tomer Cooks, Irit Allon, Orr Dimitstein, Benzion Joshua, Dexin Kong, Elena Voronov, Maurizio Scaltriti, Yaron Carmi, Cristina Conde-Lopez, Jochen Hess, Ina Kurth, Luc G. T. Morris, Pierre Saintigny, Moshe Elkabets
Summary: In head and neck cancer, treatment with MEK1/2 inhibitor delays tumor progression and enhances antitumor immunity of CD8(+) T cells. Sensitizing tumors to immunotherapy during MEK1/2 inhibition can eliminate tumors and induce immune memory. Prolonged treatment with MEK1/2 inhibitor may lead to immunosuppressive tumor microenvironment due to epithelial to mesenchymal transition.
JOURNAL FOR IMMUNOTHERAPY OF CANCER
(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, 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
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)).
Article
Chemistry, Analytical
L. Edwin Gonzalez, Lucas J. Szalwinski, Thomas C. Sams, Eric T. Dziekonski, R. Graham Cooks
Summary: The lipidomic and metabolomic profiles of sporulated and vegetative Bacillus subtilis and Bacillus thuringiensis were analyzed using a modified quadrupole ion trap mass spectrometer. The study demonstrates the effectiveness of 2D MS/MS as a rapid screening method to identify spore-forming biological agents.
ANALYTICAL CHEMISTRY
(2022)