Journal of the American Society for Mass Spectrometry最新文献_第4页

Development of an Ultrasonic Nebulization System for an Inverse Low Temperature Plasma Ionization Source. 为反向低温等离子体电离源开发超声波雾化系统。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-09-27 DOI: 10.1021/jasms.4c00259

Alexandra Pape, Juan F Ayala-Cabrera, Florian Stappert, Florian Uteschil, Cedric Thom, Shinji Yoshioka, Yasushi Terui, Oliver J Schmitz

{"title":"Development of an Ultrasonic Nebulization System for an Inverse Low Temperature Plasma Ionization Source.","authors":"Alexandra Pape, Juan F Ayala-Cabrera, Florian Stappert, Florian Uteschil, Cedric Thom, Shinji Yoshioka, Yasushi Terui, Oliver J Schmitz","doi":"10.1021/jasms.4c00259","DOIUrl":"10.1021/jasms.4c00259","url":null,"abstract":"An effective nebulization and evaporation of a liquid sample, like in liquid chromatography, mass spectrometry (LC-MS) couplings, is an essential requirement for the ionization of analyte molecules in the gas phase by, for example, atmospheric pressure chemical ionization (APCI) or the novel low temperature plasma (LTP)-based ion source. These LTP-based ion sources have recently gained interest in the field of atmospheric pressure ion sources, as they can cover a wide range of polarity and molecular mass. They can be used in combination with separation techniques like liquid chromatography or used as an ambient ion source. However, commercial nebulizer systems are of course not constructed to fit to home-built LTP-based ion sources, and this was one incentive to develop a new nebulization system. Instead of an atmospheric pressure chemical ionization (APCI) nebulizer, two commercial nebulizers were disassembled and remodeled to be used as nebulizing systems in an LC-MS setup using an LTP-based ion source. Based on these results, a novel nebulizer system was subsequently developed. To further improve the degree of ionization, cones to focus the LC eluent spray on the plasma region, heating applications, and auxiliary nitrogen gas for dispersion of the solvent droplets were implemented. The LOD that could be calculated via the rule of three resulted in an average of 2.0 μg/L for the APCI-nebulizer and 41 μg/L for the USN. Both could be reduced to 1.4 and 18 μg/L, respectively, by using a TPI-configuration instead of an iLTP. The linearity was equally good for both types of nebulization devices. The final nebulizer could also be operated with a high water content and flow rates higher than those of the two previous ones, indicating an important improvement step.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"2918-2925"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142338953","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

Photochemical and Collision-Induced Cross-Linking in Stereochemically Distinct Scaffolds of Peptides and Nitrile Imines in Gas-Phase Ions. 气相离子中肽和腈胺立体化学上不同支架的光化学和碰撞诱导交联。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-10-24 DOI: 10.1021/jasms.4c00317

Hongyi Zhu, Marianna Nytka, Tuan Ngoc Kim Vu, Karel Lemr, František Tureček

{"title":"Photochemical and Collision-Induced Cross-Linking in Stereochemically Distinct Scaffolds of Peptides and Nitrile Imines in Gas-Phase Ions.","authors":"Hongyi Zhu, Marianna Nytka, Tuan Ngoc Kim Vu, Karel Lemr, František Tureček","doi":"10.1021/jasms.4c00317","DOIUrl":"10.1021/jasms.4c00317","url":null,"abstract":"Intramolecular cross-linking between peptides and nitrile-imine intermediates was studied in stereochemically distinct conjugates in which the reacting components were mounted on cis-1,2-cyclohexane and trans-1,4-cyclohexane scaffolds that we call 1,2-s-peptides and 1,4-s-peptides, respectively. The nitrile-imine intermediates were generated by N2 loss from 2,5-diaryltetrazole tags upon UV-photodissociation at 213 and 250 nm or by collision-induced dissociation, and further interrogated by CID and UVPD-MS3. Peptide fragment ion series originating from linear structures and macrocyclic cross-links were distinguished and used to quantify the cross-linking yields. The yields in MS2 varied between 27% for AAAG conjugates to 78% for GAAAK conjugates, depending on the peptide sequence. The CID-MS3 yields were in a 57-97% range, depending on the peptide sequence. Structures of 1,2-s-peptide and 1,4-s-peptide ions as well as several of their nitrile-imine intermediates and cross-links were investigated by high-resolution cyclic ion mobility in combination with Born-Oppenheimer molecular dynamics and density functional theory calculations. Matches between the experimental and calculated collision cross sections and ion relative Gibbs energies were used to assign peptide structures. Peptide conjugates C-terminated with Gly and Lys residues underwent cross-linking by the carboxyl group, as established by MS3 sequencing and corroborated by carboxyl blocking experiments that lowered the cross-linking yields. Peptide conjugates C-terminated with Arg also cross-linked via the side-chain guanidine group. A notable feature of the 1,4-s-peptide ions was the participation of low-energy twist-boat cyclohexane conformers that was enforced by strong hydrogen bonds between the peptide and nitrile imine.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"3070-3088"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142492613","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

Leveraging Ion-Ion and Ion-Photon Activation to Improve the Sequencing of Proteins Carrying Multiple Disulfide Bonds: The Human Serum Albumin Case Study. 利用离子-离子活化和离子-光子活化改进带有多个二硫键的蛋白质测序：人类血清白蛋白案例研究。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-11-07 DOI: 10.1021/jasms.4c00391

Linda B Lieu, Joshua D Hinkle, John E P Syka, Luca Fornelli

{"title":"Leveraging Ion-Ion and Ion-Photon Activation to Improve the Sequencing of Proteins Carrying Multiple Disulfide Bonds: The Human Serum Albumin Case Study.","authors":"Linda B Lieu, Joshua D Hinkle, John E P Syka, Luca Fornelli","doi":"10.1021/jasms.4c00391","DOIUrl":"10.1021/jasms.4c00391","url":null,"abstract":"Gas-phase sequencing of large intact proteins (>30 kDa) via tandem mass spectrometry is an inherently challenging process that is further complicated by the extensive overlap of multiply charged product ion peaks, often characterized by a low signal-to-noise ratio. Disulfide bonds exacerbate this issue because of the need to cleave both the S-S and backbone bonds to liberate sequence informative fragments. Although electron-based ion activation techniques such as electron transfer dissociation (ETD) have been proven to rupture disulfide bonds in whole protein ions, they still struggle to produce extensive sequencing when multiple, concatenated S-S bonds are present on the same large polypeptide chain. Here, we evaluate the increase in sequence coverage obtained by combining activated-ion ETD (AI-ETD) and proton transfer charge reduction (PTCR) in the analysis of 66 kDa human serum albumin, which holds 17 disulfide bridges. We also describe the combination of AI-ETD with supplemental postactivation of the ETD reaction products via higher-energy collisional dissociation─a hybrid fragmentation method termed AI-EThcD. AI-EThcD leads to a further improvement compared to AI-ETD in both the global number of cleaved backbone bonds and the number of ruptured backbone bonds from disulfide-protected regions. Our results also demonstrate that the full potential of AI-ETD and AI-EThcD is unveiled only when combined with PTCR: reduction in overlap of ion signals leads to a sequence coverage as high as 39% in a single experiment, highlighting the relevance of spectral simplification in top-down mass spectrometry of large proteins.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"3265-3273"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142602811","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

Numerical Simulation of Autoresonant Ion Oscillations in an Anharmonic Electrostatic Trap. 非谐波静电陷阱中离子自共振振荡的数值模拟

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-11-07 DOI: 10.1021/jasms.4c00356

Jesús E López, Jose A Hernández, Fredy F Parada-Becerra, Carlos J Páez-González, Petr Tsygankov, Eduardo A Orozco

引用次数: 0

Obtaining 20 μm Spatial Resolution with a 2940 nm Laser by IR-MALDESI Mass Spectrometry Imaging. 通过 IR-MALDESI 质谱成像技术利用 2940 nm 激光获得 20 μm 的空间分辨率。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-11-08 DOI: 10.1021/jasms.4c00276

Seth M Eisenberg, Alena N Joignant, Kevan T Knizner, Jeffrey G Manni, David C Muddiman

引用次数: 0

Strategies for Using Postcolumn Infusion of Standards to Correct for Matrix Effect in LC-MS-Based Quantitative Metabolomics. 在基于液相色谱-质谱联用仪的定量代谢组学中使用柱后注入标准品校正基质效应的策略。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-11-15 DOI: 10.1021/jasms.4c00408

Anne-Charlotte Dubbelman, Bo van Wieringen, Lesley Roman Arias, Michael van Vliet, Roel Vermeulen, Amy C Harms, Thomas Hankemeier

{"title":"Strategies for Using Postcolumn Infusion of Standards to Correct for Matrix Effect in LC-MS-Based Quantitative Metabolomics.","authors":"Anne-Charlotte Dubbelman, Bo van Wieringen, Lesley Roman Arias, Michael van Vliet, Roel Vermeulen, Amy C Harms, Thomas Hankemeier","doi":"10.1021/jasms.4c00408","DOIUrl":"10.1021/jasms.4c00408","url":null,"abstract":"The matrix effect limits the accuracy of quantitation of the otherwise popular metabolomics technique liquid chromatography coupled to mass spectrometry (LC-MS). The gold standard to correct for this phenomenon, whereby compounds coeluting with the analyte of interest cause ionization enhancement or suppression, is to quantify an analyte based on the peak area ratio with an isotopologue added to the sample as an internal standard. However, these stable isotopes are expensive and sometimes unavailable. Here, we describe an alternative approach: matrix effect correction and quantifying analytes using a signal ratio with a postcolumn infused standard (PCIS). Using an LC-MS/MS method for eight endocannabinoids and related metabolites in plasma, we provide strategies to select, optimize, and evaluate PCIS candidates. Based on seven characteristics, the structural endocannabinoid analogue arachidonoyl-2'-fluoroethylamide was selected as a PCIS. Three methods to evaluate the PCIS correction vs no correction showed that PCIS correction improved values for the matrix effect, precision, and dilutional linearity of at least six of the analytes to within acceptable ranges. PCIS correction also resulted in parallelization of calibration curves in plasma and neat solution, for six of eight analytes even with higher accuracy than peak area ratio correction with their stable isotope labeled internal standard, i.e., the gold standard. This enables quantification based on neat solutions, which is a significant step toward absolute quantification. We conclude that PCIS has great, but so far underappreciated, potential in accurate LC-MS quantification.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"3286-3295"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11622366/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142638278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enzymatic Synthesis of Isotopically Labeled Hydrogen Peroxide for Mass Spectrometry-Based Applications. 基于质谱应用的同位素标记过氧化氢的酶法合成。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-10-04 DOI: 10.1021/jasms.4c00326

Margaret Hoare, Ruiyue Tan, Isabella Militi, Kevin A Welle, Kyle Swovick, Jennifer R Hryhorenko, Sina Ghaemmaghami

{"title":"Enzymatic Synthesis of Isotopically Labeled Hydrogen Peroxide for Mass Spectrometry-Based Applications.","authors":"Margaret Hoare, Ruiyue Tan, Isabella Militi, Kevin A Welle, Kyle Swovick, Jennifer R Hryhorenko, Sina Ghaemmaghami","doi":"10.1021/jasms.4c00326","DOIUrl":"10.1021/jasms.4c00326","url":null,"abstract":"Methionine oxidation is involved in multiple biological processes including protein misfolding and enzyme regulation. However, it is often challenging to measure levels of methionine oxidation by mass spectrometry, in part due to the prevalence of artifactual oxidation that occurs during the sample preparation and ionization steps of typical proteomic workflows. Isotopically labeled hydrogen peroxide (H218O2) can be used to block unoxidized methionines and enables accurate measurement of in vivo levels of methionine oxidation. However, H218O2 is an expensive reagent that can be difficult to obtain from commercial sources. Here, we report a method for synthesizing H218O2 in-house. Glucose oxidase catalyzes the oxidation of β-d-glucose and produces hydrogen peroxide in the process. We took advantage of this reaction to enzymatically synthesize H218O2 from 18O2 and assessed its concentration, purity, and utility in measuring methionine oxidation levels by mass spectrometry.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"3308-3312"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11622373/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370692","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Charging of DNA Complexes in Positive-Mode Native Electrospray Ionization Mass Spectrometry. 正模式原生电喷雾离子化质谱法中 DNA 复合物的电荷。

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-10-17 DOI: 10.1021/jasms.4c00335

Mia L Abramsson, Louise J Persson, Frank Sobott, Erik G Marklund, Michael Landreh

引用次数: 0

A Novel Accurate Peak Extraction Algorithm of Mass Spectrometry Based on Iterative Adaptive Curve Fitting. 基于迭代自适应曲线拟合的新型质谱峰值精确提取算法

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-10-01 DOI: 10.1021/jasms.4c00244

Fulong Deng, Xingliang He, Hanlu Yue, Hongen Sun, Bin Wu, Zhongjun Zhao, Yixiang Duan

{"title":"A Novel Accurate Peak Extraction Algorithm of Mass Spectrometry Based on Iterative Adaptive Curve Fitting.","authors":"Fulong Deng, Xingliang He, Hanlu Yue, Hongen Sun, Bin Wu, Zhongjun Zhao, Yixiang Duan","doi":"10.1021/jasms.4c00244","DOIUrl":"10.1021/jasms.4c00244","url":null,"abstract":"In the analysis of mass spectrometry, the peak identification from the overlapped region is necessary yet difficult. Although various methods have been developed to identify these peaks, especially the continuous wavelet transformation, their applications are still limited and it is hard to deal with the complex overlapped peaks. In this study, a novel peak extraction algorithm of mass spectrometry based on iterative adaptive curve fitting is proposed to address these challenges. It fully utilizes the global optimization characteristics of adaptive curve fitting. Initial peak parameters are obtained using a window searching method, and the residuals between the adaptive fitting peak and the original data indicate the fit's effectiveness and provide information about the peaks in overlap. Using this information, we performed iterative adaptive fitting, continuously updating the overlapped peaks until the residuals met the completion criteria. All of the peaks within the overlapped region can be successfully extracted by the final fitting. The proposed method is evaluated by the simulated data, the real signal from a public data set, and the spectra of two different mass spectrometry instruments. The results demonstrate that this method can more effectively extract peaks with severe overlap and multiple overlapped peaks, resist noise interference, and offer the potential to process peaks with a high dynamic range. More importantly, the proposed method accurately identifies overlapped peaks in the actual spectra from various mass spectrometry instruments, which helps the qualitative and quantitative analyses to a great extent.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"2900-2909"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142338949","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

Mobile Phase Contaminants Affect Neutral Lipid Analysis in LC-MS-Based Lipidomics Studies. 基于 LC-MS 的脂质组学研究中流动相污染物对中性脂质分析的影响

IF 3.1 2区化学

Journal of the American Society for Mass Spectrometry Pub Date : 2024-12-04 Epub Date: 2024-10-07 DOI: 10.1021/jasms.4c00320

Joshua A Roberts, Angela S Radnoff, Aleksandra Bushueva, Jocelyn A Menard, Karl V Wasslen, Meaghan Harley, Jeffrey M Manthorpe, Jeffrey C Smith

{"title":"Mobile Phase Contaminants Affect Neutral Lipid Analysis in LC-MS-Based Lipidomics Studies.","authors":"Joshua A Roberts, Angela S Radnoff, Aleksandra Bushueva, Jocelyn A Menard, Karl V Wasslen, Meaghan Harley, Jeffrey M Manthorpe, Jeffrey C Smith","doi":"10.1021/jasms.4c00320","DOIUrl":"10.1021/jasms.4c00320","url":null,"abstract":"Lipidomics is a well-established field, enabled by modern liquid chromatography mass spectrometry (LC-MS) technology, rapidly generating large amounts of data. Lipid extracts derived from biological samples are complex, and most spectral features in LC-MS lipidomics data sets remain unidentified. In-depth analyses of commercial triacylglycerol, diacylglycerol, and cholesterol ester standards revealed the expected ammoniated and sodiated ions as well as five additional unidentified higher mass peaks with relatively high intensities. The identities and origin of these unknown peaks were investigated by modifying the chromatographic mobile-phase components and LC-MS source parameters. Tandem MS (MS/MS) of each unknown adduct peak yielded no lipid structural information, producing only an intense ion of the adducted species. The unknown adducts were identified as low-mass contaminants originating from methanol and isopropanol in the mobile phase. Each contaminant was determined to be an alkylated amine species using their monoisotopic masses to calculate molecular formulas. Analysis of bovine liver extract identified 33 neutral lipids with an additional 73 alkyl amine adducts. Analysis of LC-MS-grade methanol and isopropanol from different vendors revealed substantial alkylated amine contamination in one out of three different brands that were tested. Substituting solvents for ones with lower levels of alkyl amine contamination increased lipid annotations by 36.5% or 27.4%, depending on the vendor, and resulted in >2.5-fold increases in peak area for neutral lipid species without affecting polar lipid analysis. These findings demonstrate the importance of solvent selection and disclosure for lipidomics protocols and highlight some of the major challenges when comparing data between experiments.","PeriodicalId":672,"journal":{"name":"Journal of the American Society for Mass Spectrometry","volume":" ","pages":"3095-3106"},"PeriodicalIF":3.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142379825","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