Journal of the American Society for Mass Spectrometry最新文献_第3页

Rapid Simultaneous Quantification of Four Typical Phthalate Esters in Complex Food Matrices via Thermal Desorption–Dielectric Barrier Discharge Ionization Mass Spectrometry 热解吸-介质阻挡放电电离质谱法快速同时定量复杂食品基质中四种典型邻苯二甲酸酯

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-09-28 DOI: 10.1021/jasms.6c00286

Qisen Huang, Weipeng Cai, Xiaokang Guan, Chencheng Wei, Shuxian Liu, Xiaowen Yan, Renato Zenobi

{"title":"Rapid Simultaneous Quantification of Four Typical Phthalate Esters in Complex Food Matrices via Thermal Desorption–Dielectric Barrier Discharge Ionization Mass Spectrometry","authors":"Qisen Huang, Weipeng Cai, Xiaokang Guan, Chencheng Wei, Shuxian Liu, Xiaowen Yan, Renato Zenobi","doi":"10.1021/jasms.6c00286","DOIUrl":"https://doi.org/10.1021/jasms.6c00286","url":null,"abstract":"Conventional analytical methods for detecting and quantifyingphthalateesters (PAEs) in foods generally require lengthy sample pretreatmentprocedures and suffer from severe matrix interferences. To addressthese shortcomings, a fast analytical platform based on a thermaldesorption unit that is directly interfaced with dielectric barrierdischarge ionization mass spectrometry (TD-DBDI-MS) was developed.The integration of a heated nitrogen purge system effectively suppressedatmospheric background interference and improved signal stability.Moreover, a simplified liquid–liquid extraction pretreatmentprotocol was established that eliminates the need for centrifugationand solid-phase extraction (SPE) cleanup steps. The complete analysiscycle time per sample was reduced by approximately 55% compared toconventional GC-MS/LC-MS workflows, and each analysis by TD-DBDI-MSwas completed in only 10 seconds. The method exhibited excellent linearityfor four typical PAEs in the range of 0.5–200.0 μg/Lwith correlation coefficients (R2) > 0.998. The limitsof detection (LOD) ranged from 0.11 to 0.52 μg/kg, spike recoverieswere between 82% and 106%, and relative standard deviations (RSDs)were <10%. Application to 19 commercially available food samplesrevealed widespread PAE contamination, with butyl benzyl phthalate(BBP) being detected in every sample. Contamination levels followedthe order premade dishes > milk > sugary beverages. PAE migrationlevels from plastic bag packaging were significantly higher than thosefrom plastic bottle and carton packaging. Fortunately, the measuredPAE concentrations were all well below the specific migration limits(SMLs) specified in China’s GB 5009.271-2016 regulation andEU Regulation 10/2011. This rapid, efficient, and robust method providesa novel approach for large-scale screening of PAEs in complex foodmatrices.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2598–2608"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mass Spectrometry-Based Structural Proteomics and Analytical Ultracentrifugation Characterize the Structures of Oligomeric Apolipoprotein E4 and Its Variants 基于质谱的结构蛋白质组学和分析超离心表征低聚载脂蛋白E4及其变体的结构

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-08-28 DOI: 10.1021/jasms.6c00167

Hsin-Chieh Yang, Gregory DeKoster, Berevan Baban, Carl Frieden, Michael L. Gross

{"title":"Mass Spectrometry-Based Structural Proteomics and Analytical Ultracentrifugation Characterize the Structures of Oligomeric Apolipoprotein E4 and Its Variants","authors":"Hsin-Chieh Yang, Gregory DeKoster, Berevan Baban, Carl Frieden, Michael L. Gross","doi":"10.1021/jasms.6c00167","DOIUrl":"https://doi.org/10.1021/jasms.6c00167","url":null,"abstract":"Apolipoprotein E4(ApoE4), one of the three common isoformsofApoE, differs from ApoE3 and ApoE2 by just one amino acid substitutioneach. Yet these changes in ApoE4 profoundly impact protein structureand function to make it the strongest genetic risk factor for late-onsetAlzheimer’s disease (AD). ApoE4 exhibits a tendency to formoligomers (e.g., tetramers) that complicate high-resolution structuralcharacterization in aqueous environments. Very little is known aboutthe self-associated oligomeric structures. In this study, we employedultracentrifugation, native mass spectrometry (MS), and fast photochemicaloxidation of proteins (FPOP), a mass spectrometry-based protein footprintingapproach, to investigate conformational differences among wild-typeApoE4 and two of its mutant variants ApoE4(V236E) (Jacksonville, JV)and ApoE4(V236E/L268E) (VL). These substitutions shift the oligomericequilibrium toward dimeric and monomeric states, respectively, andallow the tetramer state to be compared with the dimer and monomer.Comparative footprinting reveals that conformational changes drivenby these mutations result in altered solvent accessibility in keyregions of the protein, suggesting disruption of interfaces responsiblefor oligomerization and altered access of lipid-binding regions. GivenApoE4’s central role in lipid metabolism and its altered interactionwith lipid surfaces compared to other isoforms, these structural changeslikely modulate lipid binding affinity and may contribute to its pathologicalrole in AD. Our findings highlight the importance of conformationalstates in ApoE4 function and provide new insights into the structuralbasis of its disease-associated behavior.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2368–2378"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124870","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Serial Analyses with Mass Spectrometry Imaging Reveal Chemical and Metabolic Alterations in Liver Tissue Following Thermoembolization 质谱成像系列分析揭示热栓塞后肝组织的化学和代谢改变

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-08-28 DOI: 10.1021/jasms.6c00092

Erik N. K. Cressman, Susanne J. Lin, Erin H. Seeley

{"title":"Serial Analyses with Mass Spectrometry Imaging Reveal Chemical and Metabolic Alterations in Liver Tissue Following Thermoembolization","authors":"Erik N. K. Cressman, Susanne J. Lin, Erin H. Seeley","doi":"10.1021/jasms.6c00092","DOIUrl":"https://doi.org/10.1021/jasms.6c00092","url":null,"abstract":"Thermoembolization(TE) is a new, minimally invasive approach thatcould improve outcomes in select patients with hepatocellular carcinoma.However, little is known about the effects of this procedure at themolecular level. To gain greater insight into the molecular effectsof TE, we performed a pilot study of transarterial TE with 2-propylpentanoylchloride in a swine model with 3 animals. Liver tissues were harvested7 days after the procedure, and formalin-fixed specimens were subjectedto serial mass spectrometry imaging (MSI) analyses of metabolites,glycans, and tryptic peptides. We observed striking differences inspatial distributions for multiple features in the TE-treated anduntreated areas. Our results show that TE is highly effective in causingcoagulative necrosis in the target tissue and based on the data wepropose that TE may cause localized chemical alterations in tissues.Our study further demonstrates that MSI is a powerful tool that canprovide fundamentally new insights into the potential of using TEor other image-guided in vivo chemistry techniques to alter localbiology.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2310–2320"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149093578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Quantum Kernel Regression and Variational Quantum Regression for the CCS Prediction of Dissolved Organic Matter: A Comparative Benchmarking Study 量子核回归和变分量子回归用于溶解有机质的CCS预测：比较基准研究

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-09-10 DOI: 10.1021/jasms.6c00135

Sadollah Ebrahimi, Armand Soldera, Céline Guéguen

{"title":"Quantum Kernel Regression and Variational Quantum Regression for the CCS Prediction of Dissolved Organic Matter: A Comparative Benchmarking Study","authors":"Sadollah Ebrahimi, Armand Soldera, Céline Guéguen","doi":"10.1021/jasms.6c00135","DOIUrl":"https://doi.org/10.1021/jasms.6c00135","url":null,"abstract":"Recent advances in quantum machine learning (QML) offernew opportunitiesfor chemical property prediction, yet their practical performancerelative to established classical models remains poorly characterizedon real-world datasets. Building on our previous benchmark of classicaland deep learning models for collision cross-section (CCS) predictions,we present an empirical comparison of quantum kernel regression (QKR)and a variational quantum regressor (VQR) against classical machinelearning (CML) techniques, including Random Forest (RF), support vectorregression (SVR), Lasso, and a Voting Regressor (VR) ensemble. Usingan aquatic dissolved organic matter (DOM) dataset with five moleculardescriptors and five chemical classes, we systematically investigateQKR feature map repetitions and classical readout kernels, as wellas VQR circuit depths and optimizer choices, to identify performance-optimalQML configurations. Regression performance is evaluated using themean absolute error (MAE), root mean square error (RMSE), and coefficientof determination (R2) across training-setsizes up to 600 molecules per class. Overall, RF and Lasso deliverthe most robust CCS predictions, achieving R2 ≥ 0.9 for lignins, carbohydrates, lipids, and proteins.Meanwhile, the optimized QKR architecture exhibits substantial gainsas data increase and achieves competitive performance on chemicallyhomogeneous subsets such as carbohydrates and lipids. In contrast,the VQR ansatz remains consistently weaker than both QKR and the classicalbaselines across all classes and data sizes. The results highlightthe strong influence of dataset size, feature representation, andmolecular heterogeneity on QML performance while also identifyingconditions under which quantum methods may become competitive in futurestudies.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2321–2330"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149093539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

In Silico Top-Down Fourier Transform Mass Spectra to Advance Proteoform Analysis Methods 自顶向下的傅里叶变换质谱，以推进蛋白质形态分析方法

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-09-03 DOI: 10.1021/jasms.6c00199

Nina A. Khristenko, Konstantin O. Nagornov, Anton N. Kozhinov, David P. A. Kilgour, Yury O. Tsybin

{"title":"In Silico Top-Down Fourier Transform Mass Spectra to Advance Proteoform Analysis Methods","authors":"Nina A. Khristenko, Konstantin O. Nagornov, Anton N. Kozhinov, David P. A. Kilgour, Yury O. Tsybin","doi":"10.1021/jasms.6c00199","DOIUrl":"https://doi.org/10.1021/jasms.6c00199","url":null,"abstract":"Top-down (TD) Fourier transform mass spectrometry (FTMS)of proteinsgenerates highly information-rich mass spectra. However, the resultingspectral complexity can hinder data interpretation and method applicability.Here, we apply transient-mediated, instrument-specific simulationsof protein TD mass spectra with user-defined product ion identities.The workflow integrates sequence-based product ion generation, empiricallyinformed fragmentation statistics, charge location modeling, and user-specifiedFT processing approach. The simulations capture key FTMS characteristics,including m/z-dependent resolution,peak interference, and realistic peak shapes. As a proof of concept,we simulated carbonic anhydrase II TDMS data sets under conditionsreported for corresponding 21 T ion cyclotron resonance (ICR) FTMSelectron transfer dissociation experiments. The simulated mass spectrareproduced key experimental descriptors of spectral complexity, includingpeak density, spectral dynamic range, and isotopic structures. Usingdata sets with increasing complexity, we performed an initial evaluationof TDMS annotation performance and observed an expected decrease inproduct ion annotation rates from c-ion-only massspectra to the most complex data sets containing a-, c-, y-, and z-type product ions, reflecting the impact of spectral congestionon confident assignment. These results demonstrate that realistic in silico TDMS data sets can support systematic investigationof spectral properties in TDMS and facilitate the development andevaluation of proteoform-specific data analysis approaches. The initialdata set of simulated mass spectra and transients is available throughProteomeXchange under identifier PXD075270.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2422–2431"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149093658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Optimized Sodium-Enhanced MALDI-2 Enables Multimodal Imaging of Triacylglycerols 优化的钠增强MALDI-2使三酰基甘油的多模态成像。

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-08-25 DOI: 10.1021/jasms.6c00227

Kameron R. Molloy, Cody R. Marshall, Martin Dufresne, Lukasz G. Migas, Matthew S. Schrag, Raf Van de Plas, Jeffrey M. Spraggins

{"title":"Optimized Sodium-Enhanced MALDI-2 Enables Multimodal Imaging of Triacylglycerols","authors":"Kameron R. Molloy, Cody R. Marshall, Martin Dufresne, Lukasz G. Migas, Matthew S. Schrag, Raf Van de Plas, Jeffrey M. Spraggins","doi":"10.1021/jasms.6c00227","DOIUrl":"10.1021/jasms.6c00227","url":null,"abstract":"Triacylglycerols (TAGs) are essential neutral lipidswith criticalroles in cellular function and disease. However, spatial characterizationof these chemical species remains difficult because neutral moleculesoften exhibit low ionization efficiency with common mass spectrometry-basedimaging strategies, such as matrix-assisted laser desorption/ionizationimaging mass spectrometry (MALDI IMS). Here, we assess how ammoniumformate (AmF) or sodium carbonate buffer solution (CBS) tissue washes,combined with varying primary laser power, affect TAG sensitivitywith and without MALDI-2 postionization. We found that Na+ doping using Na+ CBS washes combined with MALDI-2 at31% total laser power was optimal for both signal intensity and molecularcoverage. Additionally, Na+ CBS-washed tissues enabledMALDI-2 to be performed using lower laser powers, making this methodcompatible with sequential microscopy experiments as part of multimodalworkflows. Applying this strategy to diseased brain tissue enabledspatial mapping of TAGs linked to Alzheimer’s disease. Thisapproach balances sensitivity and tissue preservation, providing arobust platform for multimodal spatial lipidomic studies across diversetissues and disease contexts.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2618–2622"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149035972","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Special Issue on Security and Forensic Applications of Mass Spectrometry 质谱法的安全及法医学应用特刊

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 DOI: 10.1021/jasms.6c00386

Ryan M. Bain, Glen P. Jackson

引用次数: 0

Addition of Unstructured Proline/Alanine/Serine (PAS) Tails to Folded Proteins Induces Chain Ejection Model Ionization in Native ESI-MS 非结构化脯氨酸/丙氨酸/丝氨酸（PAS）尾部在折叠蛋白上添加诱导链喷射模型电离

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-08-29 DOI: 10.1021/jasms.6c00080

Alex Listigovers, D. Andrew James, Lars Friedrich, Rebecca Walser, Arne Skerra, Derek J. Wilson

{"title":"Addition of Unstructured Proline/Alanine/Serine (PAS) Tails to Folded Proteins Induces Chain Ejection Model Ionization in Native ESI-MS","authors":"Alex Listigovers, D. Andrew James, Lars Friedrich, Rebecca Walser, Arne Skerra, Derek J. Wilson","doi":"10.1021/jasms.6c00080","DOIUrl":"https://doi.org/10.1021/jasms.6c00080","url":null,"abstract":"Denaturedand unstructured proteins have been observed to takeup high charge densities in native ESI-MS through the chain ejectionmodel (CEM). This behavior is hypothesized to originate from exposedinterior hydrophobic residues upon denaturation with nearly completeunfolding upon ejection of the protein. In this work, we demonstratethat natively unstructured, strongly hydrophilic proline/alanine/serine(PAS) sequences and even folded proteins derivatized with PAS tailscan also ionize at least partly through CEM. To determine the mechanisticorigin of hydrophilic CEM, PAS tails of different lengths were analyzedand conjugated to bovine serum albumin. The solution-phase sizes ofthe species correlate well with the size of droplets that efficientlyemit small ions through ion evaporation, thus offering a mechanismfor CEM in the absence of hydrophobicity. The charge-state distributionsand folding state of these structured/unstructured hybrids upon ionizationwere monitored by IMS-MS, showing that CEM ionization can induce partialas well as complete unfolding of folded proteins. This results inCEM-like charge acquisition and signal enhancement to an extent thatis dependent on the relative size of the natively unfolded region.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2301–2309"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Proteomic Signatures in Neuronal and Glial Cell Models of Niemann-Pick Disease Type C C型尼曼-匹克病神经元和胶质细胞模型的蛋白质组学特征

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-08-29 DOI: 10.1021/jasms.6c00184

Olivia C. Wagner, Thu T. A. Nguyen, Roshan Javanshad, Koralege C. Pathmasiri, Stephanie Boktor, Erin Davy, Wenping Li, Stephanie M. Cologna

{"title":"Proteomic Signatures in Neuronal and Glial Cell Models of Niemann-Pick Disease Type C","authors":"Olivia C. Wagner, Thu T. A. Nguyen, Roshan Javanshad, Koralege C. Pathmasiri, Stephanie Boktor, Erin Davy, Wenping Li, Stephanie M. Cologna","doi":"10.1021/jasms.6c00184","DOIUrl":"https://doi.org/10.1021/jasms.6c00184","url":null,"abstract":"Niemann-Pickdisease type C (NPC) is a lysosomal storagedisordercharacterized by the accumulation of unesterified cholesterol andglycosphingolipids in the late endosomal/lysosomal system, resultingin region-specific neurodegeneration. While the mechanism throughwhich defective NPC1 protein and thus altered cholesterol transportengenders neurodegeneration is unknown, selective reintroduction ofthe NPC1 gene in different cell types in the mouse brain can alleviatedisease symptoms, suggesting that neuronal and glial cells may playdistinct roles in disease mechanisms. Here, in an in vitro NPC model, we evaluate cell-specific changes in the proteome upontreatment with a small-molecule cholesterol-trafficking inhibitor,U18666A, which inhibits NPC1 function across three immortalized celllines in the central nervous system (CNS): mouse hippocampal neuronalcells (HT-22), mouse microglial cells (SIM-A9), and human hybridizedoligodendrocytes (MO3.13). Using nanoliquid chromatography–massspectrometry (LC–MS) techniques, we observe 21 common proteinsupregulated in all U18666A-treated cells. We also note that markersof activated microglia were significantly altered in SIM-A9 microglialcells, whereas cytoskeletal and membrane-related proteins were elevatedin MO3.13. In HT-22 hippocampal neuronal cells, we identify proteinchanges associated with altered glucose metabolism and postulate thatATP-citrate lyase (ACLY), a protein central to multiple biologicalpathways, might play a role in responding to aberrant cholesteroltrafficking and metabolism in NPC.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2396–2409"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124853","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhancing Ion Yields in MALDI-2-MSI Using Dopant-Assisted Post Ionization for High-Resolution MS-Imaging of Lipids and Metabolites 利用掺杂剂辅助后电离提高MALDI-2-MSI的离子产量，用于脂质和代谢物的高分辨率质谱成像

IF 2.9 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2026-10-07 Epub Date: 2026-09-23 DOI: 10.1021/jasms.6c00149

Christoph Bookmeyer, Alexander Potthoff, Benedikt Stauff, Klaus Dreisewerd, Jens Soltwisch

{"title":"Enhancing Ion Yields in MALDI-2-MSI Using Dopant-Assisted Post Ionization for High-Resolution MS-Imaging of Lipids and Metabolites","authors":"Christoph Bookmeyer, Alexander Potthoff, Benedikt Stauff, Klaus Dreisewerd, Jens Soltwisch","doi":"10.1021/jasms.6c00149","DOIUrl":"https://doi.org/10.1021/jasms.6c00149","url":null,"abstract":"Matrix-assisted laser desorption ionization mass spectrometryimaging(MALDI-MSI) is the most widely used label-free method for mappingthe molecular distribution of lipids and metabolites from tissue sectionsand cell cultures. To mitigate the problem of partially low MALDIion yields for several of these analyte classes, different post ionizationtechniques have recently been developed─for example, MALDI-2,where a second UV-laser pulse intersects the initial particle plumeto generate additional charges. Here, we show that the MALDI-2 signalintensities of important analyte classes can be further increasedupon introducing reactive dopant vapor into the MALDI-2 ion source.Dopant assistance as an optional add-on was realized in prototypeform on MALDI-2 ion sources of a Spectroglyph Injector-Orbitrap MSIsetup and a timsTOF fleX MALDI-2 instrument. Acetone, anisole, toluene,2-propanol, and chlorobenzene were tested as dopants. Acetone provedto be the most effective and robust dopant for the given setup andMALDI matrix, and thus was used for further parameter optimizationon both instruments. We demonstrate that with dopant-assisted (DA-)MALDI-2,a signal increase of up to 5 orders of magnitude, as compared to regularMALDI, is, for instance, achieved for several classes of sterols,glycerophospholipids, and sphingolipids. Next to the increased intensityof signals for abundant lipids, the total amount of annotated signals(based on MS1) was also majorly increased by the use of dopants. Wedemonstrate the potential for biomedical imaging applications withthe examples of murine spleen and cerebellum sections, analyzed inthe positive- and negative-ion mode.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":"37 10","pages":"2331–2340"},"PeriodicalIF":2.9,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149093573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0