Journal of Mass Spectrometry最新文献

{"title":"Prototyping an ionization source for non-engineers","authors":"Kevan T. Knizner,&nbsp;Seth M. Eisenberg,&nbsp;David C. Muddiman","doi":"10.1002/jms.4995","DOIUrl":"10.1002/jms.4995","url":null,"abstract":"<p>Novel mass spectrometry (MS) based analytical platforms have enabled scientists to detect and quantify molecules within biological and environmental samples more accurately. Novel MS instrumentation starts as a prototype and, after years of development, can become a commercial product to be used by the larger MS community. Without the initial prototype, many MS-based instruments today would not be produced. Additionally, biotechnology companies are the main drivers for research, development, and production of novel instruments, but the tools for prototyping instrumentation have never been more accessible. Here, we present a tutorial on prototyping instrumentation through the case study of developing the Next Generation IR-MALDESI source to show that an engineering degree is not required to design and construct a prototype instrument with modern hardware and software. We discuss the prototyping process, the necessary skills required for efficient prototyping, and information about common hardware and software used within initial prototypes.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/jms.4995","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138830138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Performance of collagen-based matrices from Nile tilapia skin: A pilot proteomic study in a murine model of wound healing","authors":"Cláudia B. A. Medeiros,&nbsp;Iasmim Lopes de Lima,&nbsp;Thiago Barbosa Cahú,&nbsp;Bruna R. Muniz,&nbsp;Maria Helena M. L. Ribeiro,&nbsp;Érico Higino de Carvalho,&nbsp;Marcos Nogueira Eberlin,&nbsp;Marcelo J. B. Miranda,&nbsp;Ranilson de Souza Bezerra,&nbsp;Roberto Afonso da Silva,&nbsp;José Luiz de Lima Filho","doi":"10.1002/jms.4988","DOIUrl":"10.1002/jms.4988","url":null,"abstract":"<p>Full-thickness cutaneous trauma, due to the lack of dermis, leads to difficulty in epithelialization by keratinocytes, developing a fibrotic scar, with less elasticity than the original skin, which may have disorders in predisposed individuals, resulting in hypertrophic scar and keloids. Biomedical materials have excellent characteristics, such as good biocompatibility and low immunogenicity, which can temporarily replace traditional materials used as primary dressings. In this work, we developed two dermal matrices based on Nile tilapia collagen, with (M_GAG) and without (M) glycosaminoglycans, using a sugarcane polymer membrane as a matrix support. To assess the molecular mechanisms driving wound healing, we performed qualitative proteomic analysis on the wound bed in an in vivo study involving immunocompetent murine models at 14 and 21 days post-full-thickness skin injury. Gene Ontology and Pathway analysis revealed that both skins were markedly represented by modulation of the immune system, emphasizing controlling the acute inflammation response at 14 and 21 days post-injury. Furthermore, both groups showed significant enrichment of pathways related to RNA and protein metabolism, suggesting an increase in protein synthesis required for tissue repair and proper wound closure. Other pathways, such as keratinization and vitamin D3 metabolism, were also enriched in the groups treated with M matrix. Finally, both matrices improved wound healing in a full post-thick skin lesion. However, our preliminary molecular data reveals that the collagen-mediated healing matrix lacking glycosaminoglycan (M) exhibited a phenotype more favorable to tissue repair, making it more suitable for use before skin grafts.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138717353","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"LC–MS/MS analysis of coccidiostats in meat supply chain safety","authors":"Claudia Ancillotti,&nbsp;Lisa Bonciani,&nbsp;Davide Passerini,&nbsp;Giulia Scanavini,&nbsp;Roberto Riccio","doi":"10.1002/jms.4993","DOIUrl":"10.1002/jms.4993","url":null,"abstract":"<p>The presence of coccidiostats in meat products represents an important topic because of the animal administration of these substances, authorized as feed additives for targeted species, in order to prevent and inhibit coccidiosis. Coccidiostats include both ionophores and synthetic molecules characterized by different chemical–physical properties such as polarity. Meat is a matrix characterized by many interfering compound groups, such as proteins, phospholipids, and fats. High-performance liquid chromatography (HPLC) coupled to mass spectrometry (MS) analysis allows the required selectivity and sensitivity for discriminating analytes and matrix interferences.</p><p>For these reasons, an LC–MS/MS method for the analysis of coccidiostats in meat products was developed without SPE purification steps. The correct analyte quantification is allowed by matrix-matched calibration. The method validation was performed by the replicated analysis of spiked meat samples at two different concentration levels (limit of quantification—LOQ—and a 10 times LOQ) in order to evaluate method recovery and repeatability, plus spiked samples at higher concentrations up to 10,000 μg/kg. Moreover, the metrological approach was used for the calculation of method uncertainty. The application of the developed method to real samples evidenced the presence of some non-ionophores coccidiostats in the meat and liver of chicken and rabbit species. Although, the determined concentration was below the established MRLs, the monitoring of coccidiostats in the meat supply chain is confirmed as a good strategy in order to safeguard consumer health.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138717351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Advancing the analytical toolkit in the investigation of vector mosquito host biting site selection","authors":"Madelien Wooding,&nbsp;Tyren Dodgen,&nbsp;Egmont R. Rohwer,&nbsp;Yvette Naudé","doi":"10.1002/jms.4992","DOIUrl":"10.1002/jms.4992","url":null,"abstract":"<p>High-resolution mass spectrometry and ion mobility spectrometry provide additional confidence in biological marker discovery and elucidation by adding additional peak capacity through physiochemical separation orthogonal to chromatography. Sophisticated analytical techniques have proved valuable in the identification of human skin surface chemicals used by vector mosquitoes to find their human host. Polydimethylsiloxane (PDMS) was used as a non-invasive passive wearable sampler to concentrate skin surface non-volatile and semi-volatile compounds prior to solvent desorption directly in an LC vial, thereby simplifying the link between extraction and analysis. Ultra-performance liquid chromatography with ion mobility spectrometry coupled with high-resolution mass spectrometry (UPLC-IMS-HRMS) was used for compound separation and detection. A comparison of the skin chemical profiles between the ankle and wrist skin surface region sampled over a 5-day period for a human volunteer was done. Twenty-three biomarkers were tentatively identified with the aid of a collision cross-section (CCS) prediction tool, seven associated with the ankle skin surface region and 16 closely associated with the wrist skin surface. Ten amino acids were detected and unequivocally identified on the human skin surface for the first time. Furthermore, 22 previously unreported skin surface compounds were tentatively identified on the human skin surface using accurate mass, CCS values and fragmentation patterns. Method limits of detection for the passive skin sampling method ranged from 8.7 (sulfadimethoxine) to 95 ng (taurine). This approach enabled the detection and identification of as-yet unknown human skin surface compounds and provided corresponding CCS values.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://analyticalsciencejournals.onlinelibrary.wiley.com/doi/epdf/10.1002/jms.4992","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138717509","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A new absolute quantitative method for peptide and metabolite detection","authors":"Carlo Brogna,&nbsp;Simone Cristoni","doi":"10.1002/jms.4991","DOIUrl":"10.1002/jms.4991","url":null,"abstract":"<p>Mass spectrometry is widely employed in various analytical fields for both compound identification and quantification. While in the case of compound identification, the high-resolution instrument has increased selectivity and characterization efficiency; in the case of quantitative analysis, some critical tasks actually remain. In particular, different compounds exhibit different ionization efficiency, and this introduces the need to have a calibration standard for each analyte. In this paper, we present a new elaborative data technology, which makes it possible to standardize calibration between different instruments and molecules, making it absolute. The method was applied to data acquired by means of liquid chromatography mass spectrometry by means of an ion trap analyzer. The approach is based on the correlation of the ion trap space charge effect and the analyte concentration. The method was validated in the analysis of compounds having different polarity: hydrossitirosol, arginine, thyodiglicolic acid, and a peptide mixture of bacteria cultures derived the human gut microbiome where was found poliovirus. Moreover, it was used to obtain the absolute quantitation of peptides originating from the tryptic digestion of bacterial proteins in the fecal samples. It was therefore possible to identify and quantify different derived bacterial proteins of the poliomyelitis virus coded in bacteria derived from the gastrointestinal tract.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138717348","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Software-assisted automated detection and identification of “unknown” fentanyl analogues","authors":"Eyal Drug,&nbsp;Dana Marder,&nbsp;Iris Binyamin,&nbsp;Dina Yeffet,&nbsp;Eytan Gershonov,&nbsp;Shai Dagan","doi":"10.1002/jms.4994","DOIUrl":"10.1002/jms.4994","url":null,"abstract":"<p>Fentanyl and its non-pharmaceutical analogues (NPFs) are potent synthetic opioids, traditionally used for pain management, with ever-increasing illicit uses. Tightening the regulation for known fentanyls leads to new synthetic analogues in the opioid market. Furthermore, the Organization for the Prohibition of Chemical Weapons (OPCW) has recently issued a decision regarding aerosolized use of central nervous system (CNS)-acting agents, such as fentanyl and its analogues, under the concern that these materials could be misused for terror or war purposes. The ever-increasing development of new fentanyl analogues makes the task of detection and identification of these new, unknown analogues crucial. In this work, we introduce an automated tool for the detection and putative identification of “unknown” fentanyl analogues, using liquid chromatography–mass spectrometry (LC–MS) (high-resolution mass spectrometry [HRMS]) analysis, subsequently followed by data processing using the “Compound Discoverer” software. This software, in our modified use, enabled the automatic detection of various fentanyl analogues, by “digging” out components and comparing them to pre-calculated theoretical molecular ions of possible modifications or transformations on the fentanyl backbone structure (no library or database used). Subsequently, structural elucidation for the proposed component of interest is carried out by automated MS/MS data interpretation, as performed by the software. This method was explored on 12 fentanyl-based “unknown” analogues used as model examples, including chemical modifications such as fluorination and methylation. In all tested compounds, automatic detection and identification were achieved, even at concentrations as low as 1 ng/mL in an environmental soil matrix extract.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138717345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"An analytical approach for on-site analysis of breath samples for Δ9-tetrahydrocannabinol (THC)","authors":"Jack Henion,&nbsp;Changtong Hao,&nbsp;Daniel Eikel,&nbsp;Olof Beck,&nbsp;Peter Stambeck","doi":"10.1002/jms.4987","DOIUrl":"https://doi.org/10.1002/jms.4987","url":null,"abstract":"<p>Increased acceptance of cannabis containing the psychoactive component, Δ9-tetrahydrocannabinol (THC), raises concerns about the potential for impaired drivers and increased highway accidents. In contrast to the “breathalyzer” test, which is generally accepted for determining the alcohol level in a driver, there is no currently accepted roadside test for THC in a motorist. There is a need for an easily collectible biological sample from a potentially impaired driver coupled with an accurate on-site test to measure the presence and quantity of THC in a driver. A novel breath collection device is described, which includes three separate sample collectors for collecting identical A, B, and C breath samples from a subject. A simple one-step ethanol extraction of the “A” breath collector sample can be analyzed by UHPLC/selected ion monitoring (SIM) liquid chromatography/mass spectrometry (LC/MS) to provide qualitative and quantitative determination of THC in breath sample in less than 4 min for samples collected up to 6 h after smoking a cannabis cigarette. SIM LC/MS bioanalyses employed d3-THC as the stable isotope internal standard fortified in negative control breath samples for quantitation including replicates of six calibrator standards and three quality control (QC) samples. Subsequent confirmation of the same breath sample in the B collectors was then confirmed by a reference lab by LC/MS/MS analysis. Fit-for-purpose bioanalytical validation consistent with pharmaceutical regulated bioanalyses produced pharmacokinetic (PK) curves for the two volunteer cannabis smokers. These results produced PK curves, which showed a rapid increase of THC in the breath of the subjects in the first hour followed by reduced THC levels in the later time points. A simpler single-point calibration curve procedure with calibrators and QC prepared in ethanol provided similar results. Limitations to this approach include the higher cost and operator skill sets for the instrumentation employed and the inability to actually determine driver impairment.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138739727","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Characterization of isomeric acetyl amino acids and di-acetyl amino acids by LC/MS/MS","authors":"Addipilli Ramunaidu,&nbsp;Pallerla Pavankumar,&nbsp;Nagarjunachary Ragi,&nbsp;Rodda Ramesh,&nbsp;Medicharla V. Jagannatham,&nbsp;Prabhakar Sripadi","doi":"10.1002/jms.4982","DOIUrl":"10.1002/jms.4982","url":null,"abstract":"<p>Acetylation of amino acids is important in the molecular biology and biochemistry because they are part of several metabolic pathways. N-acetyl amino acids can form through degradation of N-acetyl proteins or direct acetylation of amino acids by specific enzymes. Acetylation of α-amino acids can be either on the alpha –NH₂ or on the side-chain functional group, where both the acetyl products are isomeric and can show different biological roles. Theoretically, all proteinogenic α-amino acids are expected to undergo acetylation and they can be a part of metabolome. Thus, it is essential to detect and identify all the possible acetylated products of α-amino acids for untargeted metabolomics studies. In this study, it is aimed to synthesize and characterize all acetylated products of natural α-amino acids. A total of 20 N_α-acetyl amino acids (<b>1</b>–<b>20</b>), six side-chain acetyl amino acids (<b>21</b>–<b>26</b>), and six diacetyl amino acids (<b>27</b>–<b>32</b>) were synthesized and characterized by liquid chromatography-electrospray ionizationtandem mass spectrometry (LC–ESI–MS/MS). The [M + H]⁺ ions of all the acetyl amino acids were subjected to MS/MS experiments to obtain their structural information. Apart from the expected loss of (H₂O + CO) (immonium ions), most of the acetyl amino acids specifically showed loss of H₂O and loss of a ketene (C₂H₂O) from [M+H]⁺ ions. The side-chain acetyl amino acids showed a clear-cut structure specific fragment ions that enabled easy differentiation from their isomeric N_α-acetyl amino acids. The other isomeric/isobaric acetyl amino acids could also be easily distinguished by their MS/MS spectra. The MS/MS of immonium ions of the acetyl amino acids were also studied, and they included characteristic products reflecting the structures of parent N_α-acetyl and side-chain acetyl amino acids.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138460371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Modelling some rod set imperfections of a quadrupole mass filter","authors":"Pavel V. Bugrov,&nbsp;Aleksey A. Sysoev,&nbsp;Nikolai V. Konenkov","doi":"10.1002/jms.4986","DOIUrl":"10.1002/jms.4986","url":null,"abstract":"<p>The problem of modeling the mass peak shape of a quadrupole mass filter (QMF) with round rods is considered. A number of factors leading to the degradation of the mass peak shape are studied, namely, displacement of the electrodes with respect to their original position, changes in the diameter of the electrodes, and asymmetry of the supply potentials. Decomposition of the rod set field on multipole fields allows to obtain an analytical representation of the ion motion equations. Simulations have shown that a parallel shift of one or two electrodes leads to a shift of the peak along the mass number axis and dips at the peak apex. Unbalance of supply voltages does not significantly distort the peak shape, but it shifts the peak along the mass axis and creates a jump of the quadrupole offset potential proportional to the relative unbalance <math>\u0000 <mo>∆</mo>\u0000 <mi>V</mi>\u0000 <mo>/</mo>\u0000 <mi>V</mi></math> of X and Y rods potentials.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138291108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Further exploration of the collision-induced dissociation of select beta blockers: Acebutolol, atenolol, bisoprolol, carteolol, and labetalol","authors":"Matthew J. Carlo,&nbsp;Amanda L. Patrick","doi":"10.1002/jms.4985","DOIUrl":"10.1002/jms.4985","url":null,"abstract":"<p>Beta blockers are a class of drugs commonly used to treat heart-related diseases; they are also regulated under the World Anti-Doping Agency. Tandem mass spectrometry is often used in the pharmaceutical industry, clinical analysis laboratory, and antidoping laboratory for detection and characterization of drugs and their metabolites. A deeper chemical understanding of dissociation pathways may eventually lead to an improved ability to predict tandem mass spectra of compounds based strictly on their chemical structure (or vice versa), which is especially important for characterization of unknowns such as emerging designer drugs or novel metabolites. In addition to providing insights into dissociation pathways, the use of energy-resolved breakdown curves can produce improved selectivity and lend insights into optimal fragmentation conditions for liquid chromatography-tandem mass spectrometry LC–MS/MS workflows. Here, we perform energy-resolved collision cell and multistage ion trap collision-induced dissociation-mass spectrometry (CID-MS) experiments, along with complementary density functional theory calculations, on five beta blockers (acebutolol, atenolol, bisoprolol, carteolol, and labetalol), to better understand the details of the pathways giving rise to the observed MS/MS patterns. Results from this work are contextualized within previously reported literature on these compounds. New insights into the formation of the characteristic product ion <i>m/z</i> 116 and the pathway leading to characteristic loss of 77 u are highlighted. We also present comparisons of breakdown curves obtained via qToF, quadrupole ion trap, and in-source CID, allowing for differences between the data to be noted and providing a step toward allowing for improved selectivity of breakdown curves to be realized on simple instruments such as single quadrupoles or ion traps.</p>","PeriodicalId":16178,"journal":{"name":"Journal of Mass Spectrometry","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2023-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138291107","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}