Tyrosine phosphorylation is a crucial posttranslational modification that is involved in various aspects of cell biology and often has functions in cancers. It is necessary not only to identify the specific phosphorylation sites but also to quantify their phosphorylation levels under specific pathophysiological conditions. Because of its high sensitivity and accuracy, mass spectrometry (MS) has been widely used to identify endogenous and synthetic phosphotyrosine proteins/peptides across a range of biological systems. However, phosphotyrosine-containing proteins occur in extremely low abundance and they degrade easily, severely challenging the application of MS. This review highlights the advances in both quantitative analysis procedures and enrichment approaches to tyrosine phosphorylation before MS analysis and reviews the differences among phosphorylation, sulfation, and nitration of tyrosine residues in proteins. In-depth insights into tyrosine phosphorylation in a wide variety of biological systems will offer a deep understanding of how signal transduction regulates cellular physiology and the development of tyrosine phosphorylation-related drugs as cancer therapeutics.
酪氨酸磷酸化是一种重要的翻译后修饰,涉及细胞生物学的各个方面,通常在癌症中发挥作用。不仅需要确定特定的磷酸化位点,还需要量化其在特定病理生理条件下的磷酸化水平。由于质谱法(MS)具有高灵敏度和准确性,因此已被广泛用于鉴定一系列生物系统中的内源性和合成磷酸酪氨酸蛋白/肽。然而,含磷酪氨酸的蛋白质含量极低,而且容易降解,这对质谱的应用提出了严峻的挑战。本综述重点介绍了 MS 分析前酪氨酸磷酸化定量分析程序和富集方法的进展,并回顾了蛋白质中酪氨酸残基的磷酸化、硫酸化和硝酸化之间的差异。深入了解各种生物系统中的酪氨酸磷酸化,将有助于深入理解信号转导如何调节细胞生理以及开发酪氨酸磷酸化相关药物作为癌症疗法。
{"title":"Mass spectrometry analysis of phosphotyrosine-containing proteins","authors":"Jiajia Li, Xianquan Zhan","doi":"10.1002/mas.21836","DOIUrl":"10.1002/mas.21836","url":null,"abstract":"<p>Tyrosine phosphorylation is a crucial posttranslational modification that is involved in various aspects of cell biology and often has functions in cancers. It is necessary not only to identify the specific phosphorylation sites but also to quantify their phosphorylation levels under specific pathophysiological conditions. Because of its high sensitivity and accuracy, mass spectrometry (MS) has been widely used to identify endogenous and synthetic phosphotyrosine proteins/peptides across a range of biological systems. However, phosphotyrosine-containing proteins occur in extremely low abundance and they degrade easily, severely challenging the application of MS. This review highlights the advances in both quantitative analysis procedures and enrichment approaches to tyrosine phosphorylation before MS analysis and reviews the differences among phosphorylation, sulfation, and nitration of tyrosine residues in proteins. In-depth insights into tyrosine phosphorylation in a wide variety of biological systems will offer a deep understanding of how signal transduction regulates cellular physiology and the development of tyrosine phosphorylation-related drugs as cancer therapeutics.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"43 4","pages":"857-887"},"PeriodicalIF":6.6,"publicationDate":"2023-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10716510","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}
David Smith, Patrik Španěl, Nicholas Demarais, Vaughan S. Langford, Murray J. McEwan
Selected ion flow tube mass spectrometry (SIFT-MS) is now recognized as the most versatile analytical technique for the identification and quantification of trace gases down to the parts-per-trillion by volume, pptv, range. This statement is supported by the wide reach of its applications, from real-time analysis, obviating sample collection of very humid exhaled breath, to its adoption in industrial scenarios for air quality monitoring. This review touches on the recent extensions to the underpinning ion chemistry kinetics library and the alternative challenge of using nitrogen carrier gas instead of helium. The addition of reagent anions in the Voice200 series of SIFT-MS instruments has enhanced the analytical capability, thus allowing analyses of volatile trace compounds in humid air that cannot be analyzed using reagent cations alone, as clarified by outlining the anion chemistry involved. Case studies are reviewed of breath analysis and bacterial culture volatile organic compound (VOC), emissions, environmental applications such as air, water, and soil analysis, workplace safety such as transport container fumigants, airborne contamination in semiconductor fabrication, food flavor and spoilage, drugs contamination and VOC emissions from packaging to demonstrate the stated qualities and uniqueness of the new generation SIFT-MS instrumentation. Finally, some advancements that can be made to improve the analytical capability and reach of SIFT-MS are mentioned.
{"title":"Recent developments and applications of selected ion flow tube mass spectrometry (SIFT-MS)","authors":"David Smith, Patrik Španěl, Nicholas Demarais, Vaughan S. Langford, Murray J. McEwan","doi":"10.1002/mas.21835","DOIUrl":"10.1002/mas.21835","url":null,"abstract":"<p>Selected ion flow tube mass spectrometry (SIFT-MS) is now recognized as the most versatile analytical technique for the identification and quantification of trace gases down to the parts-per-trillion by volume, pptv, range. This statement is supported by the wide reach of its applications, from real-time analysis, obviating sample collection of very humid exhaled breath, to its adoption in industrial scenarios for air quality monitoring. This review touches on the recent extensions to the underpinning ion chemistry kinetics library and the alternative challenge of using nitrogen carrier gas instead of helium. The addition of reagent anions in the <i>Voice200</i> series of SIFT-MS instruments has enhanced the analytical capability, thus allowing analyses of volatile trace compounds in humid air that cannot be analyzed using reagent cations alone, as clarified by outlining the anion chemistry involved. Case studies are reviewed of breath analysis and bacterial culture volatile organic compound (VOC), emissions, environmental applications such as air, water, and soil analysis, workplace safety such as transport container fumigants, airborne contamination in semiconductor fabrication, food flavor and spoilage, drugs contamination and VOC emissions from packaging to demonstrate the stated qualities and uniqueness of the new generation SIFT-MS instrumentation. Finally, some advancements that can be made to improve the analytical capability and reach of SIFT-MS are mentioned.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"44 2","pages":"101-134"},"PeriodicalIF":6.9,"publicationDate":"2023-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/mas.21835","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10774108","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}
Jürgen Claesen, Alan Rockwood, Mikhail Gorshkov, Dirk Valkenborg
The isotope distribution, which reflects the number and probabilities of occurrence of different isotopologues of a molecule, can be theoretically calculated. With the current generation of (ultra)-high-resolution mass spectrometers, the isotope distribution of molecules can be measured with high sensitivity, resolution, and mass accuracy. However, the observed isotope distribution can differ substantially from the expected isotope distribution. Although differences between the observed and expected isotope distribution can complicate the analysis and interpretation of mass spectral data, they can be helpful in a number of specific applications. These applications include, yet are not limited to, the identification of peptides in proteomics, elucidation of the elemental composition of small organic molecules and metabolites, as well as wading through peaks in mass spectra of complex bioorganic mixtures such as petroleum and humus. In this review, we give a nonexhaustive overview of factors that have an impact on the observed isotope distribution, such as elemental isotope deviations, ion sampling, ion interactions, electronic noise and dephasing, centroiding, and apodization. These factors occur at different stages of obtaining the isotope distribution: during the collection of the sample, during the ionization and intake of a molecule in a mass spectrometer, during the mass separation and detection of ionized molecules, and during signal processing.
{"title":"The isotope distribution: A rose with thorns","authors":"Jürgen Claesen, Alan Rockwood, Mikhail Gorshkov, Dirk Valkenborg","doi":"10.1002/mas.21820","DOIUrl":"10.1002/mas.21820","url":null,"abstract":"<p>The isotope distribution, which reflects the number and probabilities of occurrence of different isotopologues of a molecule, can be theoretically calculated. With the current generation of (ultra)-high-resolution mass spectrometers, the isotope distribution of molecules can be measured with high sensitivity, resolution, and mass accuracy. However, the observed isotope distribution can differ substantially from the expected isotope distribution. Although differences between the observed and expected isotope distribution can complicate the analysis and interpretation of mass spectral data, they can be helpful in a number of specific applications. These applications include, yet are not limited to, the identification of peptides in proteomics, elucidation of the elemental composition of small organic molecules and metabolites, as well as wading through peaks in mass spectra of complex bioorganic mixtures such as petroleum and humus. In this review, we give a nonexhaustive overview of factors that have an impact on the observed isotope distribution, such as elemental isotope deviations, ion sampling, ion interactions, electronic noise and dephasing, centroiding, and apodization. These factors occur at different stages of obtaining the isotope distribution: during the collection of the sample, during the ionization and intake of a molecule in a mass spectrometer, during the mass separation and detection of ionized molecules, and during signal processing.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"44 1","pages":"22-42"},"PeriodicalIF":6.9,"publicationDate":"2023-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11624904/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10644535","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}
Jacob D. Guthrie, Caroline E. R. Rowell, Ruth O. Anyaeche, Kawthar Z. Alzarieni, Hilkka I. Kenttämaa
Biomass-derived degraded lignin and cellulose serve as possible alternatives to fossil fuels for energy and chemical resources. Fast pyrolysis of lignocellulosic biomass generates bio-oil that needs further refinement. However, as pyrolysis causes massive degradation to lignin and cellulose, this process produces very complex mixtures. The same applies to degradation methods other than fast pyrolysis. The ability to identify the degradation products of lignocellulosic biomass is of great importance to be able to optimize methodologies for the conversion of these mixtures to transportation fuels and valuable chemicals. Studies utilizing tandem mass spectrometry have provided invaluable, molecular-level information regarding the identities of compounds in degraded biomass. This review focuses on the molecular-level characterization of fast pyrolysis and other degradation products of lignin and cellulose via tandem mass spectrometry based on collision-activated dissociation (CAD). Many studies discussed here used model compounds to better understand both the ionization chemistry of the degradation products of lignin and cellulose and their ions' CAD reactions in mass spectrometers to develop methods for the structural characterization of the degradation products of lignocellulosic biomass. Further, model compound studies were also carried out to delineate the mechanisms of the fast pyrolysis reactions of lignocellulosic biomass. The above knowledge was used to assign likely structures to many degradation products of lignocellulosic biomass.
{"title":"Characterization of the degradation products of lignocellulosic biomass by using tandem mass spectrometry experiments, model compounds, and quantum chemical calculations","authors":"Jacob D. Guthrie, Caroline E. R. Rowell, Ruth O. Anyaeche, Kawthar Z. Alzarieni, Hilkka I. Kenttämaa","doi":"10.1002/mas.21832","DOIUrl":"10.1002/mas.21832","url":null,"abstract":"<p>Biomass-derived degraded lignin and cellulose serve as possible alternatives to fossil fuels for energy and chemical resources. Fast pyrolysis of lignocellulosic biomass generates bio-oil that needs further refinement. However, as pyrolysis causes massive degradation to lignin and cellulose, this process produces very complex mixtures. The same applies to degradation methods other than fast pyrolysis. The ability to identify the degradation products of lignocellulosic biomass is of great importance to be able to optimize methodologies for the conversion of these mixtures to transportation fuels and valuable chemicals. Studies utilizing tandem mass spectrometry have provided invaluable, molecular-level information regarding the identities of compounds in degraded biomass. This review focuses on the molecular-level characterization of fast pyrolysis and other degradation products of lignin and cellulose via tandem mass spectrometry based on collision-activated dissociation (CAD). Many studies discussed here used model compounds to better understand both the ionization chemistry of the degradation products of lignin and cellulose and their ions' CAD reactions in mass spectrometers to develop methods for the structural characterization of the degradation products of lignocellulosic biomass. Further, model compound studies were also carried out to delineate the mechanisms of the fast pyrolysis reactions of lignocellulosic biomass. The above knowledge was used to assign likely structures to many degradation products of lignocellulosic biomass.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"43 2","pages":"369-408"},"PeriodicalIF":6.6,"publicationDate":"2023-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/mas.21832","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10607615","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}
Voislav Blagojevic, Gregory K. Koyanagi, Diethard K. Böhme
The evolution and applications of flow tube mass spectrometry in the study of catalysis promoted by atomic metal ions are tracked from the pioneering days in Boulder, Colorado, to the construction and application of the ICP/SIFT/QqQ and ESI/qQ/SIFT/QqQ instruments at York University and the VISTA-SIFT instrument at the Air Force Research Laboratory. The physical separation of various sources of atomic metal ions from the flow tube in the latter instruments facilitates the spatial resolution of redox reactions and allows the separate measurement of the kinetics of both legs of a two-step catalytic cycle, while also allowing a view of the catalytic cycle in progress downstream in the reaction region of the flow tube. We focus on measurements on O-atom transfer and bond activation catalysis as first identified in Boulder and emphasize fundamental aspects such as the thermodynamic window of opportunity for catalysis, catalytic efficiency, and computed energy landscapes for atomic metal cation catalysis. Gas-phase applications include: the catalytic oxidation of CO to CO2, of H2 to H2O, and of C2H4 to CH3CHO all with N2O as the source of oxygen; the catalytic oxidation of CH4 to CH3OH with O3; the catalytic oxidation of C6H6 with O2. We also address the environmentally important catalytic reduction of NO2 and NO to N2 with CO and H2 by catalytic coupling of two-step catalytic cycles in a multistep cycle. Overall, the power of atomic metal cations in catalysis, and the use of flow tube mass spectrometry in revealing this power, is clearly demonstrated.
从科罗拉多州博尔德的开创时期,到约克大学的 ICP/SIFT/QqQ 和 ESI/qQ/SIFT/QqQ 仪器以及空军研究实验室的 VISTA-SIFT 仪器的建造和应用,跟踪了流管质谱法在原子金属离子催化研究中的演变和应用。在后一种仪器中,各种原子金属离子源与导流管的物理分离有助于提高氧化还原反应的空间分辨率,并能分别测量两步催化循环中两段的动力学,同时还能观察导流管反应区下游正在进行的催化循环。我们的重点是测量在博尔德首次发现的 O 原子转移和键活化催化,并强调催化的热力学机会窗口、催化效率和原子金属阳离子催化的计算能谱等基本方面。气相应用包括:以 N2 O 作为氧源,催化 CO 氧化为 CO2、H2 氧化为 H2 O 和 C2 H4 氧化为 CH3 CHO;以 O3 催化 CH4 氧化为 CH3 OH;以 O2 催化 C6 H6 氧化。我们还通过多步循环中两步催化循环的催化耦合,解决了将 NO2 和 NO 与 CO 和 H2 催化还原为 N2 的重要环境问题。总之,我们清楚地展示了原子金属阳离子在催化过程中的威力,以及使用流动管质谱法揭示这种威力的方法。
{"title":"Probing gas phase catalysis by atomic metal cations with flow tube mass spectrometry","authors":"Voislav Blagojevic, Gregory K. Koyanagi, Diethard K. Böhme","doi":"10.1002/mas.21831","DOIUrl":"10.1002/mas.21831","url":null,"abstract":"<p>The evolution and applications of flow tube mass spectrometry in the study of catalysis promoted by atomic metal ions are tracked from the pioneering days in Boulder, Colorado, to the construction and application of the ICP/SIFT/QqQ and ESI/qQ/SIFT/QqQ instruments at York University and the VISTA-SIFT instrument at the Air Force Research Laboratory. The physical separation of various sources of atomic metal ions from the flow tube in the latter instruments facilitates the spatial resolution of redox reactions and allows the separate measurement of the kinetics of both legs of a two-step catalytic cycle, while also allowing a view of the catalytic cycle in progress downstream in the reaction region of the flow tube. We focus on measurements on O-atom transfer and bond activation catalysis as first identified in Boulder and emphasize fundamental aspects such as the thermodynamic window of opportunity for catalysis, catalytic efficiency, and computed energy landscapes for atomic metal cation catalysis. Gas-phase applications include: the catalytic oxidation of CO to CO<sub>2</sub>, of H<sub>2</sub> to H<sub>2</sub>O, and of C<sub>2</sub>H<sub>4</sub> to CH<sub>3</sub>CHO all with N<sub>2</sub>O as the source of oxygen; the catalytic oxidation of CH<sub>4</sub> to CH<sub>3</sub>OH with O<sub>3</sub>; the catalytic oxidation of C<sub>6</sub>H<sub>6</sub> with O<sub>2</sub>. We also address the environmentally important catalytic reduction of NO<sub>2</sub> and NO to N<sub>2</sub> with CO and H<sub>2</sub> by catalytic coupling of two-step catalytic cycles in a multistep cycle. Overall, the power of atomic metal cations in catalysis, and the use of flow tube mass spectrometry in revealing this power, is clearly demonstrated.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"44 2","pages":"154-184"},"PeriodicalIF":6.9,"publicationDate":"2023-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10590419","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}
Leena R. Pade, Kaitlyn E. Stepler, Erika P. Portero, Kellen DeLaney, Peter Nemes
Biological processes unfold across broad spatial and temporal dimensions, and measurement of the underlying molecular world is essential to their understanding. Interdisciplinary efforts advanced mass spectrometry (MS) into a tour de force for assessing virtually all levels of the molecular architecture, some in exquisite detection sensitivity and scalability in space-time. In this review, we offer vignettes of milestones in technology innovations that ushered sample collection and processing, chemical separation, ionization, and 'omics analyses to progressively finer resolutions in the realms of tissue biopsies and limited cell populations, single cells, and subcellular organelles. Also highlighted are methodologies that empowered the acquisition and analysis of multidimensional MS data sets to reveal proteomes, peptidomes, and metabolomes in ever-deepening coverage in these limited and dynamic specimens. In pursuit of richer knowledge of biological processes, we discuss efforts pioneering the integration of orthogonal approaches from molecular and functional studies, both within and beyond MS. With established and emerging community-wide efforts ensuring scientific rigor and reproducibility, spatiotemporal MS emerged as an exciting and powerful resource to study biological systems in space-time.
{"title":"Biological mass spectrometry enables spatiotemporal ‘omics: From tissues to cells to organelles","authors":"Leena R. Pade, Kaitlyn E. Stepler, Erika P. Portero, Kellen DeLaney, Peter Nemes","doi":"10.1002/mas.21824","DOIUrl":"10.1002/mas.21824","url":null,"abstract":"<p>Biological processes unfold across broad spatial and temporal dimensions, and measurement of the underlying molecular world is essential to their understanding. Interdisciplinary efforts advanced mass spectrometry (MS) into a tour de force for assessing virtually all levels of the molecular architecture, some in exquisite detection sensitivity and scalability in space-time. In this review, we offer vignettes of milestones in technology innovations that ushered sample collection and processing, chemical separation, ionization, and 'omics analyses to progressively finer resolutions in the realms of tissue biopsies and limited cell populations, single cells, and subcellular organelles. Also highlighted are methodologies that empowered the acquisition and analysis of multidimensional MS data sets to reveal proteomes, peptidomes, and metabolomes in ever-deepening coverage in these limited and dynamic specimens. In pursuit of richer knowledge of biological processes, we discuss efforts pioneering the integration of orthogonal approaches from molecular and functional studies, both within and beyond MS. With established and emerging community-wide efforts ensuring scientific rigor and reproducibility, spatiotemporal MS emerged as an exciting and powerful resource to study biological systems in space-time.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"43 1","pages":"106-138"},"PeriodicalIF":6.6,"publicationDate":"2023-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9086082","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}
This review encompasses guided ion beam tandem mass spectrometry studies of hydrated metal dication complexes. Metals include the Group 2 alkaline earths (Mg, Ca, Sr, and Ba), late first-row transition metals (Mn, Fe, Co, Ni, Cu, and Zn), along with Cd. In all cases, threshold collision-induced dissociation experiments are used to quantitatively determine the sequential hydration energies for M2+(H2O)x complexes ranging in size from one to 11 water molecules. Periodic trends in these bond dissociation energies are examined and discussed. Values are compared to other experimental results when available. In addition to dissociation by simple water ligand loss, complexes at a select size (which differs from metal to metal) are also observed to undergo charge separation to yield a hydrated metal hydroxide cation and a hydrated proton. This leads to the concept of a critical size, xcrit, and the periodic trends in this value are also discussed.
{"title":"Periodic trends in the hydration energies and critical sizes of alkaline earth and transition metal dication water complexes","authors":"Fan Yang, P. B. Armentrout","doi":"10.1002/mas.21830","DOIUrl":"10.1002/mas.21830","url":null,"abstract":"<p>This review encompasses guided ion beam tandem mass spectrometry studies of hydrated metal dication complexes. Metals include the Group 2 alkaline earths (Mg, Ca, Sr, and Ba), late first-row transition metals (Mn, Fe, Co, Ni, Cu, and Zn), along with Cd. In all cases, threshold collision-induced dissociation experiments are used to quantitatively determine the sequential hydration energies for M<sup>2+</sup>(H<sub>2</sub>O)<sub><i>x</i></sub> complexes ranging in size from one to 11 water molecules. Periodic trends in these bond dissociation energies are examined and discussed. Values are compared to other experimental results when available. In addition to dissociation by simple water ligand loss, complexes at a select size (which differs from metal to metal) are also observed to undergo charge separation to yield a hydrated metal hydroxide cation and a hydrated proton. This leads to the concept of a critical size, <i>x</i><sub>crit</sub>, and the periodic trends in this value are also discussed.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"44 2","pages":"135-153"},"PeriodicalIF":6.9,"publicationDate":"2023-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9095396","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}
{"title":"A special issue honoring Prof. Hilkka Kenttämaa for her contributions to the field of mass spectrometry","authors":"Edouard Niyonsaba","doi":"10.1002/mas.21833","DOIUrl":"10.1002/mas.21833","url":null,"abstract":"","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"43 2","pages":"233-234"},"PeriodicalIF":6.6,"publicationDate":"2023-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10513254","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}
The intact-mass MS measurements are becoming increasingly popular in characterization of a range of biopolymers, especially those of interest to biopharmaceutical industry. However, as the complexity of protein therapeutics and other macromolecular medicines increases, the new challenges arise, one of which is the high levels of structural heterogeneity that are frequently exhibited by such products. The very notion of the molecular mass measurement loses its clear and intuitive meaning when applied to an extremely heterogenous system that cannot be characterized by a unique mass, but instead requires that a mass distribution be considered. Furthermore, convoluted mass distributions frequently give rise to unresolved ionic signal in mass spectra, from which little-to-none meaningful information can be extracted using standard approaches that work well for homogeneous systems. However, a range of technological advances made in the last decade, such as the hyphenation of intact-mass MS measurements with front-end separations, better integration of ion mobility in MS workflows, development of an impressive arsenal of gas-phase ion chemistry tools to supplement MS methods, as well as the revival of the charge detection MS and its triumphant entry into the field of bioanalysis already made impressive contributions towards addressing the structural heterogeneity challenge. An overview of these techniques is accompanied by critical analysis of the strengths and weaknesses of different approaches, and a brief overview of their applications to specific classes of biopharmaceutical products, vaccines, and nonbiological complex drugs.
{"title":"Mass spectrometry-based methods to characterize highly heterogeneous biopharmaceuticals, vaccines, and nonbiological complex drugs at the intact-mass level","authors":"Igor A. Kaltashov, Daniil G. Ivanov, Yang Yang","doi":"10.1002/mas.21829","DOIUrl":"10.1002/mas.21829","url":null,"abstract":"<p>The intact-mass MS measurements are becoming increasingly popular in characterization of a range of biopolymers, especially those of interest to biopharmaceutical industry. However, as the complexity of protein therapeutics and other macromolecular medicines increases, the new challenges arise, one of which is the high levels of structural heterogeneity that are frequently exhibited by such products. The very notion of the molecular mass measurement loses its clear and intuitive meaning when applied to an extremely heterogenous system that cannot be characterized by a unique mass, but instead requires that a mass distribution be considered. Furthermore, convoluted mass distributions frequently give rise to unresolved ionic signal in mass spectra, from which little-to-none meaningful information can be extracted using standard approaches that work well for homogeneous systems. However, a range of technological advances made in the last decade, such as the hyphenation of intact-mass MS measurements with front-end separations, better integration of ion mobility in MS workflows, development of an impressive arsenal of gas-phase ion chemistry tools to supplement MS methods, as well as the revival of the charge detection MS and its triumphant entry into the field of bioanalysis already made impressive contributions towards addressing the structural heterogeneity challenge. An overview of these techniques is accompanied by critical analysis of the strengths and weaknesses of different approaches, and a brief overview of their applications to specific classes of biopharmaceutical products, vaccines, and nonbiological complex drugs.</p>","PeriodicalId":206,"journal":{"name":"Mass Spectrometry Reviews","volume":"43 1","pages":"139-165"},"PeriodicalIF":6.6,"publicationDate":"2022-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10081043","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}
Alexander J. Grooms, Benjamin J. Burris, Abraham K. Badu-Tawiah
Chemical analysis by analytical instrumentation has played a major role in disease diagnosis, which is a necessary step for disease treatment. While the treatment process often targets specific organs or compounds, the diagnostic step can occur through various means, including physical or chemical examination. Chemically, the genome may be evaluated to give information about potential genetic outcomes, the transcriptome to provide information about expression actively occurring, the proteome to offer insight on functions causing metabolite expression, or the metabolome to provide a picture of both past and ongoing physiological function in the body. Mass spectrometry (MS) has been elevated among other analytical instrumentation because it can be used to evaluate all four biological machineries of the body. In addition, MS provides enhanced sensitivity, selectivity, versatility, and speed for rapid turnaround time, qualities that are important for instance in clinical procedures involving the diagnosis of a pediatric patient in intensive care or a cancer patient undergoing surgery. In this review, we provide a summary of the use of MS to evaluate biomarkers for newborn screening and cancer diagnosis. As many reviews have recently appeared focusing on MS methods and instrumentation for metabolite analysis, we sought to describe the biological basis for many metabolomic and additional omics biomarkers used in newborn screening and how tandem MS methods have recently been applied, in comparison to traditional methods. Similar comparison is done for cancer screening, with emphasis on emerging MS approaches that allow biological fluids, tissues, and breath to be analyzed for the presence of diagnostic metabolites yielding insight for treatment options based on the understanding of prior and current physiological functions of the body.
分析仪器的化学分析在疾病诊断中发挥了重要作用,而疾病诊断是疾病治疗的必要步骤。治疗过程通常以特定器官或化合物为目标,而诊断步骤则可以通过各种方式进行,包括物理或化学检查。在化学方面,可以对基因组进行评估,以了解潜在的遗传结果;对转录组进行评估,以了解正在进行的表达;对蛋白质组进行评估,以了解导致代谢物表达的功能;或对代谢组进行评估,以了解体内过去和现在的生理功能。质谱(MS)在其他分析仪器中的地位较高,因为它可用于评估人体的所有四种生物机制。此外,质谱还具有更高的灵敏度、选择性、多功能性和快速反应能力,这些特性在临床诊断重症监护中的儿科病人或手术中的癌症病人时非常重要。在这篇综述中,我们总结了如何利用 MS 评估用于新生儿筛查和癌症诊断的生物标记物。由于最近出现了许多以代谢物分析 MS 方法和仪器为重点的综述,我们试图描述新生儿筛查中使用的许多代谢组学和其他 omics 生物标记物的生物学基础,以及与传统方法相比,串联 MS 方法最近是如何应用的。我们还对癌症筛查进行了类似的比较,重点介绍了新出现的 MS 方法,这些方法可以分析生物液体、组织和呼吸中是否存在诊断性代谢物,从而根据对人体先前和当前生理功能的了解来选择治疗方案。
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