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Electrospray Ionization Mass Spectrometry of Apolipoprotein CIII to Evaluate O-glycan Site Occupancy and Sialylation in Congenital Disorders of Glycosylation. 利用载脂蛋白 CIII 的电喷雾离子化质谱法评估先天性糖基化紊乱的 O-聚糖位点占用率和 Sialylation。
Mass spectrometry Pub Date : 2022-01-01 Epub Date: 2022-08-10 DOI: 10.5702/massspectrometry.A0104
Yoshinao Wada, Nobuhiko Okamoto
{"title":"Electrospray Ionization Mass Spectrometry of Apolipoprotein CIII to Evaluate <i>O</i>-glycan Site Occupancy and Sialylation in Congenital Disorders of Glycosylation.","authors":"Yoshinao Wada, Nobuhiko Okamoto","doi":"10.5702/massspectrometry.A0104","DOIUrl":"10.5702/massspectrometry.A0104","url":null,"abstract":"<p><p>Congenital disorders of glycosylation (CDG) are inherited metabolic diseases that affect the synthesis of glycoconjugates. Defects in mucin-type <i>O</i>-glycosylation occur independently or in combination with <i>N</i>-glycosylation disorders, and the profiling of the <i>O</i>-glycans of apolipoprotein CIII (apoCIII) by mass spectrometry (MS) can be used to support a diagnosis. The biomarkers are site occupancy and sialylation levels, which are indicated by the content of non-glycosylated apoCIII0a isoform and by the ratio of monosialylated apoCIII1 to disialylated apoCIII2 isoforms, respectively. In this report, electrospray ionization (ESI) quadrupole MS of apoCIII was used to identify these biomarkers. Among the instrumental parameters, the declustering potential (DP) induced the fragmentation of the <i>O</i>-glycan moiety including the Thr-GalNAc linkage, resulting in an increase in apoCIII0a ions. This incurs the risk of creating a false positive for reduced site occupancy. The apoCIII1/apoCIII2 ratio was substantially unchanged despite some dissociation of sialic acids. Therefore, appropriate DP settings are especially important when transferrin, which requires a higher DP, for <i>N</i>-glycosylation disorders is analyzed simultaneously with apoCIII in a single ESI MS measurement. Finally, a reference range of diagnostic biomarkers and mass spectra of apoCIII obtained from patients with SLC35A1-, TRAPPC11-, and ATP6V0A2-CDG are presented.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":" ","pages":"A0104"},"PeriodicalIF":0.0,"publicationDate":"2022-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9396207/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"40346745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrospray Ionization Mass Spectrometry of Transferrin: Use of Quadrupole Mass Analyzers for Congenital Disorders of Glycosylation. 转铁蛋白的电喷雾电离质谱分析:四极杆质谱分析仪用于先天性糖基化疾病。
Mass spectrometry Pub Date : 2022-01-01 Epub Date: 2022-04-15 DOI: 10.5702/massspectrometry.A0103
Yoshinao Wada, Nobuhiko Okamoto
{"title":"Electrospray Ionization Mass Spectrometry of Transferrin: Use of Quadrupole Mass Analyzers for Congenital Disorders of Glycosylation.","authors":"Yoshinao Wada,&nbsp;Nobuhiko Okamoto","doi":"10.5702/massspectrometry.A0103","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0103","url":null,"abstract":"<p><p>Electrospray ionization (ESI) mass spectrometry of transferrin can be used to diagnose congenital disorders of glycosylation (CDG) by detecting abnormal <i>N</i>-glycosylation due to reduced site occupancy or processing failure. Time-of-flight mass spectrometers are widely used to separate 25-45 charged ions in the <i>m</i>/<i>z</i> 1,700-3,000 range, and a summed zero-charge mass distribution is generated despite the risk of improper deconvolution. In this study, the low <i>m</i>/<i>z</i> region of the multiply-charged ion mass spectrum enabled a robust analysis of CDG. A triple quadrupole mass spectrometer, the standard instrument for newborn screening for inborn errors of metabolism, permitted the identification of the key ions characteristic of different types of CDG affecting <i>PMM2</i>, <i>ALG14</i>, <i>SLC35A1</i>, <i>SLC35A2</i>, <i>MAN1B1</i> and <i>PGM1</i> in the <i>m</i>/<i>z</i> 1,970-2,000 region. Charge deconvolution was used as a complementary tool for validating the findings. It was necessary to set a cutoff level for the evaluation, since small peaks indicating glycosylation failure or reduced sialylation were observed, even in control subjects. This method and workflow facilitates the implementation of MS-based analyses and the screening of CDG in clinical laboratories.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":" ","pages":"A0103"},"PeriodicalIF":0.0,"publicationDate":"2022-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9395324/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"40346746","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 3
Improvement in Ionization Efficiency Using Metal Oxide Nanoparticles in Laser Desorption/Ionization Mass Spectrometry of a Cancer Drug. 金属氧化物纳米粒子在抗癌药物激光解吸/电离质谱分析中提高电离效率。
Mass spectrometry Pub Date : 2021-01-01 Epub Date: 2021-12-23 DOI: 10.5702/massspectrometry.A0099
Hiroki Kannen, Yuto Miyoshi, Hisanao Hazama, Kunio Awazu
{"title":"Improvement in Ionization Efficiency Using Metal Oxide Nanoparticles in Laser Desorption/Ionization Mass Spectrometry of a Cancer Drug.","authors":"Hiroki Kannen,&nbsp;Yuto Miyoshi,&nbsp;Hisanao Hazama,&nbsp;Kunio Awazu","doi":"10.5702/massspectrometry.A0099","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0099","url":null,"abstract":"<p><p>Mass spectrometry imaging (MSI) without labeling has the potential for faster screening in drug development. Matrix-assisted laser desorption/ionization (MALDI) is typically used, but it has a large matrix size and uneven drug distribution. Surface-assisted laser desorption/ionization (SALDI) using nanoparticles (NPs) may overcome these issues. Here, the influence of NPs, solvent ratio, and order of dropping of NPs on SALDI-MSI of protoporphyrin IX (PpIX), a cancer drug, are reported. A solution of PpIX in a 50% aqueous solution of 50% acetonitrile at a concentration of 10 μM was used. The NPs include ZnO, Fe<sub>3</sub>O<sub>4</sub>, and four types of TiO<sub>2</sub>. The NPs were fabricated by dissolving them on an aqueous 90% acetonitrile solution. Mass spectra were obtained with a time-of-flight mass spectrometer using a Nd:YAG laser at a 355-nm wavelength. The signal intensity using TiO<sub>2</sub> at a 0.5 mg/mL concentration in 50% acetonitrile was increased by 1.6-fold compared to that without TiO<sub>2</sub>. Changing the solvent to 90% acetonitrile gave a uniform TiO<sub>2</sub> distribution and a 9-fold increase in the signal intensity for PpIX. Among the four types of TiO<sub>2</sub> with different particle sizes and crystal structures, TiO<sub>2</sub> with a smaller particle size and a rutile crystal structure produced the highest signal intensity. Forming a layer on top of the PpIX also resulted in an increased signal intensity. Hence, SALDI using TiO<sub>2</sub> provides effective ionization of the drug. In the future, we plan to investigate a spray method for the ionization of PpIX using TiO<sub>2</sub> for the MSI of various drugs.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"10 1","pages":"A0099"},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8697360/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39792149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Gas-Phase Adsorption of N2 on Protonated Molecules and Its Application to the Structural Elucidation of Small Molecules. 质子化分子对N2的气相吸附及其在小分子结构解析中的应用。
Mass spectrometry Pub Date : 2021-01-01 Epub Date: 2021-06-10 DOI: 10.5702/massspectrometry.A0096
Hiromori Murashima, Akimasa Fujihara
{"title":"Gas-Phase Adsorption of N<sub>2</sub> on Protonated Molecules and Its Application to the Structural Elucidation of Small Molecules.","authors":"Hiromori Murashima,&nbsp;Akimasa Fujihara","doi":"10.5702/massspectrometry.A0096","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0096","url":null,"abstract":"<p><p>The gas-phase adsorption of N<sub>2</sub> on protonated serine (Ser, C<sub>3</sub>H<sub>7</sub>NO<sub>3</sub>), threonine (Thr, C<sub>4</sub>H<sub>9</sub>NO<sub>3</sub>), glycine (Gly, C<sub>2</sub>H<sub>5</sub>NO<sub>2</sub>), and 2-aminoethanol (C<sub>2</sub>H<sub>7</sub>NO) was investigated using a tandem mass spectrometer equipped with an electrospray ionization source and a cold ion trap. N<sub>2</sub> molecules were adsorbed on the free X-H (X=O and N) groups of protonated molecules. Gas-phase N<sub>2</sub> adsorption-mass spectrometry detected the presence of free X-H groups in the molecular structures, and was applied to the structural elucidation of small molecules. When the 93 structures with an elemental composition of C<sub>3</sub>H<sub>7</sub>NO<sub>3</sub> were filtered using the gas-phase N<sub>2</sub> adsorption-mass spectrometry results for Ser, the number of possible molecular structures was reduced to 8 <i>via</i> the quantification of the X-H groups. Restricting and minimizing the number of possible candidates were effective steps in the structural elucidation process. Gas-phase N<sub>2</sub> adsorption-mass spectrometry combined with mass spectrometry-based techniques has the potential for being useful for elucidating the molecular structures of a variety of molecules.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"10 1","pages":"A0096"},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8188007/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39238233","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
A Method for Expanding Mass Range on a Multi-Turn Time-of-Flight Mass Spectrometer by a Lap Superimposed Spectrum. 一种用搭接叠加谱扩展多转飞行时间质谱仪质量范围的方法。
Mass spectrometry Pub Date : 2021-01-01 Epub Date: 2021-10-14 DOI: 10.5702/massspectrometry.A0098
Toshinobu Hondo, Michisato Toyoda
{"title":"A Method for Expanding Mass Range on a Multi-Turn Time-of-Flight Mass Spectrometer by a Lap Superimposed Spectrum.","authors":"Toshinobu Hondo,&nbsp;Michisato Toyoda","doi":"10.5702/massspectrometry.A0098","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0098","url":null,"abstract":"<p><p>A time-of-flight mass spectrometer that uses a closed-orbit flight path can achieve a high mass resolving power and a high mass accuracy with a small instrument footprint. It has long been known that a drawback to a closed flight path is an obtained spectrum may contain peaks by ions at a different number of laps. A lower <i>m</i>/<i>z</i> ion may overtake higher <i>m</i>/<i>z</i> ions, resulting in the peak being superimposed on an acquired mass spectrum; therefore, such a mass bandwidth of the analyzer is limited to a narrow range given the current situation. However, recent research has documented a solution to the problem based on careful study of the equation of motion of an ion in a closed-path analyzer. All of the ions in the analyzer remain in motion in orbit by the nature of the closed flight path, thus resulting in a superimposed spectrum with the width of the orbital period of the highest mass in the sample matrix, which contains several different lap numbers. When target ions for the sample are known in advance, the time-of-flight for a given <i>m</i>/<i>z</i> can be determined regardless of the lap number under given analyzer conditions, and peak assignment can be self-validated by comparison to a mass spectrum acquired at a different lap condition. Furthermore, the <i>m</i>/<i>z</i> value for an unknown ion can also be determined by comparing time-of-flight values on spectra acquired at different lap conditions.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"10 1","pages":"A0098"},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8514288/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39563876","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Corona Discharge and Field Electron Emission in Ambient Air Using a Sharp Metal Needle: Formation and Reactivity of CO3 -• and O2 -•. 环境空气中使用锋利金属针的电晕放电和场电子发射:CO3 -•和O2 -•的形成和反应性。
Mass spectrometry Pub Date : 2021-01-01 Epub Date: 2021-12-25 DOI: 10.5702/massspectrometry.A0100
Kenzo Hiraoka, Stephanie Rankin-Turner, Satoshi Ninomiya, Haruo Shimada, Kazumasa Kinoshita, Shinichi Yamabe
{"title":"Corona Discharge and Field Electron Emission in Ambient Air Using a Sharp Metal Needle: Formation and Reactivity of CO<sub>3</sub> <sup>-•</sup> and O<sub>2</sub> <sup>-•</sup>.","authors":"Kenzo Hiraoka,&nbsp;Stephanie Rankin-Turner,&nbsp;Satoshi Ninomiya,&nbsp;Haruo Shimada,&nbsp;Kazumasa Kinoshita,&nbsp;Shinichi Yamabe","doi":"10.5702/massspectrometry.A0100","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0100","url":null,"abstract":"<p><p>CO<sub>3</sub> <sup>-•</sup> and O<sub>2</sub> <sup>-•</sup> are known to be strong oxidizing reagents in biological systems. CO<sub>3</sub> <sup>-•</sup> in particular can cause serious damage to DNA and proteins by H<sup>•</sup> abstraction reactions. However, H<sup>•</sup> abstraction of CO<sub>3</sub> <sup>-•</sup> in the gas phase has not yet been reported. In this work we report on gas-phase ion/molecule reactions of CO<sub>3</sub> <sup>-•</sup> and O<sub>2</sub> <sup>-•</sup> with various molecules. CO<sub>3</sub> <sup>-•</sup> was generated by the corona discharge of an O<sub>2</sub> reagent gas using a cylindrical tube ion source. O<sub>2</sub> <sup>-•</sup> was generated by the application of a 15 kHz high frequency voltage to a sharp needle in ambient air at the threshold voltage for the appearance of an ion signal. In the reactions of CO<sub>3</sub> <sup>-•</sup>, a decrease in signal intensities of CO<sub>3</sub> <sup>-•</sup> accompanied by the simultaneous increase of that of HCO<sub>3</sub> <sup>-</sup> was observed when organic compounds with H-C bond energies lower than ∼100 kcal mol<sup>-1</sup> such as <i>n</i>-hexane, cyclohexane, methanol, ethanol, 1-propanol, 2-propanol, and toluene were introduced into the ion source. This clearly indicates the occurrence of H<sup>•</sup> abstraction. O<sub>2</sub> <sup>-•</sup> abstracts H<sup>+</sup> from acid molecules such as formic, acetic, trifluoroacetic, nitric and amino acids. Gas-phase CO<sub>3</sub> <sup>-•</sup> may play a role as a strong oxidizing reagent as it does in the condensed phase. The major discharge product CO<sub>3</sub> <sup>-•</sup> in addition to O<sub>2</sub> <sup>-•</sup>, O<sub>3</sub>, and NO <i><sub>x</sub> <sup>•</sup></i> that are formed in ambient air may cause damage to biological systems.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"10 1","pages":"A0100"},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8697365/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39792150","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effect of Phosphorylation on the Collision Cross Sections of Peptide Ions in Ion Mobility Spectrometry 离子迁移谱法中磷酸化对肽离子碰撞截面的影响
Mass spectrometry Pub Date : 2020-06-15 DOI: 10.1101/2020.06.15.151639
Kosuke Ogata, Chih-Hsiang Chang, Y. Ishihama
{"title":"Effect of Phosphorylation on the Collision Cross Sections of Peptide Ions in Ion Mobility Spectrometry","authors":"Kosuke Ogata, Chih-Hsiang Chang, Y. Ishihama","doi":"10.1101/2020.06.15.151639","DOIUrl":"https://doi.org/10.1101/2020.06.15.151639","url":null,"abstract":"The insertion of ion mobility spectrometry (IMS) between LC and MS can improve peptide identification in both proteomics and phosphoproteomics by providing structural information that is complementary to LC and MS, because IMS separates ions on the basis of differences in their shapes and charge states. However, it is necessary to know how phosphate groups affect the peptide collision cross sections (CCS) in order to accurately predict phosphopeptide CCS values and to maximize the usefulness of IMS. In this work, we systematically characterized the CCS values of 4,433 pairs of mono-phosphopeptide and corresponding unphosphorylated peptide ions using trapped ion mobility spectrometry (TIMS). Nearly one-third of the mono-phosphopeptide ions evaluated here showed smaller CCS values than their unphosphorylated counterparts, even though phosphorylation results in a mass increase of 80 Da. Significant changes of CCS upon phosphorylation occurred mainly in structurally extended peptides with large numbers of basic groups, possibly reflecting intramolecular interactions between phosphate and basic groups.","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"33 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2020-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79253559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 8
Temperature-Resolved Proton Transfer Reactions of Biomolecular Ions. 生物分子离子的温度分辨质子转移反应。
Mass spectrometry Pub Date : 2020-01-01 Epub Date: 2020-03-31 DOI: 10.5702/massspectrometry.A0083
Shinji Nonose
{"title":"Temperature-Resolved Proton Transfer Reactions of Biomolecular Ions.","authors":"Shinji Nonose","doi":"10.5702/massspectrometry.A0083","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0083","url":null,"abstract":"<p><p>Temperature-resolved proton transfer reactions of multiply-protonated angiotensin I, disulfide-intact and -reduced lysozyme, and ubiquitin ions to primary, secondary and aromatic amines were examined in the gas phase. Absolute reaction rate constants for the proton transfer were determined from the intensities of the parent and product ions in mass spectra. Dramatic changes were observed in the distribution of product ions and the reaction rate constants. In particular, the rate constants for disulfide-intact lysozyme ions changed more drastically with the change in charge state and temperature compared to the corresponding values for disulfide-reduced ions. Proton transfer reactions were enhanced or suppressed as the result of the formation of complexes between the ions with gaseous molecules, which is related to changes in their conformation with changing.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"9 1","pages":"A0083"},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7242783/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38057401","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Analytical Capability of High-Time Resolution-Multiple Collector-Inductively Coupled Plasma-Mass Spectrometry for the Elemental and Isotopic Analysis of Metal Nanoparticles. 高时间分辨率-多重收集器-电感耦合等离子体质谱法分析金属纳米颗粒元素和同位素的能力。
Mass spectrometry Pub Date : 2020-01-01 Epub Date: 2020-06-12 DOI: 10.5702/massspectrometry.A0085
Takafumi Hirata, Shuji Yamashita, Mirai Ishida, Toshihiro Suzuki
{"title":"Analytical Capability of High-Time Resolution-Multiple Collector-Inductively Coupled Plasma-Mass Spectrometry for the Elemental and Isotopic Analysis of Metal Nanoparticles.","authors":"Takafumi Hirata,&nbsp;Shuji Yamashita,&nbsp;Mirai Ishida,&nbsp;Toshihiro Suzuki","doi":"10.5702/massspectrometry.A0085","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0085","url":null,"abstract":"<p><p>We measured the Re/Os (<sup>185</sup>Re/<sup>188</sup>Os) and <sup>187</sup>Os/<sup>188</sup>Os ratios from nanoparticles (NPs) using a multiple collector-inductively coupled plasma-mass spectrometer equipped with high-time resolution ion counters (HTR-MC-ICP-MS). Using the HTR-MC-ICP-MS system developed in this study, the simultaneous data acquisition of four isotopes was possible with a time resolution of up to 10 μs. This permits the quantitative analysis of four isotopes to be carried out from transient signals (<i>e.g.</i>, <0.6 ms) emanating from the NPs. Iridium-Osmium NPs were produced from a naturally occurring Ir-Os alloy (ruthenosmiridium from Hokkaido, Japan; osmiridium from British Columbia, Canada; iridosmine from the Urals region of Russia) through a laser ablation technique, and the resulting nanoparticles were collected by bubbling water through a suspension. The <sup>187</sup>Os/<sup>188</sup>Os ratios for individual NPs varied significantly, mainly due to the counting statistics of the <sup>187</sup>Os and <sup>188</sup>Os signals. Despite the large variation in the measured ratios, the resulting <sup>187</sup>Os/<sup>188</sup>Os ratios for three Ir-Os bearing minerals, were 0.121±0.013 for Hokkaido, 0.110±0.012 for British Columbia, and 0.122±0.020 for the Urals, and these values were in agreement with the ratios obtained by the conventional laser ablation-MC-ICP-MS technique. The data obtained here provides a clear demonstration that the HTR-MC-ICP-MS technique can become a powerful tool for monitoring elemental and isotope ratios from NPs of multiple components.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"9 1","pages":"A0085"},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7291549/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"38109445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 7
Kendrick Analysis and Complex Isotopic Patterns: A Case Study of the Compositional Analysis of Pristine and Heated Polybrominated Flame Retardants by High-Resolution MALDI Mass Spectrometry. Kendrick分析和复杂同位素模式:用高分辨率MALDI质谱分析原始和加热多溴系阻燃剂的成分。
Mass spectrometry Pub Date : 2020-01-01 Epub Date: 2020-02-06 DOI: 10.5702/massspectrometry.A0079
Sayaka Nakamura, Hiroaki Sato, Thierry N J Fouquet
{"title":"Kendrick Analysis and Complex Isotopic Patterns: A Case Study of the Compositional Analysis of Pristine and Heated Polybrominated Flame Retardants by High-Resolution MALDI Mass Spectrometry.","authors":"Sayaka Nakamura,&nbsp;Hiroaki Sato,&nbsp;Thierry N J Fouquet","doi":"10.5702/massspectrometry.A0079","DOIUrl":"https://doi.org/10.5702/massspectrometry.A0079","url":null,"abstract":"<p><p>The Kendrick analysis is used for the processing and visualization of mass spectra obtained from polymers containing C, H, O and/or Si with simple isotopic patterns (monoisotope=lightest isotope=most intense isotope for short chains). In the case of heteroatoms with complex isotopic patterns, the impact of the chosen isotope on point alignments in Kendrick plots has not been examined extensively. Rich isotopic patterns also make the evaluation of the mass and nature of the repeating unit and end-groups more difficult from the mass spectrum in the case of unknown samples due to the number of peaks and the absence of a monoisotopic peak. Using a polybrominated polycarbonate as running example, we report that horizontal point alignments can be obtained in a Kendrick plot using the mass of the most abundant isotope instead of the monoisotopic mass as is usually done. Rotating the plot (\"reverse Kendrick analysis\") helps to accurately evaluate the mass of the most abundant isotope of the repeating unit, as well as the nature of the brominated neutral expelled upon gentle heating (debromination or dehydrobromination). The whole procedure is then applied to the characterization of an unknown polybrominated flame retardant in an industrial formulation before and after heating.</p>","PeriodicalId":18243,"journal":{"name":"Mass spectrometry","volume":"9 1","pages":"A0079"},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7039712/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"37726939","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 2
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