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  • MASS SPECTROMETRY FOR A HOLISTIC VIEW OF NATURAL EXTRACTS OF PHYTOTHERAPEUTIC INTEREST
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2020-01-12
    Laura Moracci; Pietro Traldi; Marco Agostini

    In the study of natural products new strategies which favor a holistic approach, integrating the traditional reductionist methods usually employed, have been proposed. In this frame, the studies carried out by us in the last decade show that fingerprints, mainly obtained by electrospray ionization mass spectrometry (ESI‐MS), lead to the characterization of natural extracts from different botanical species but also of phytotherapeutic products constituted by mixtures of extracts from different plants. Laser desorption ionization and matrix‐assisted laser desorption ionization techniques were also employed and by the use of different matrices some complementary results were achieved. Results obtained by standard spectrophotometric and liquid chromatography methods were compared with those achieved by direct infusion of the extract in ESI‐MS conditions, indicating an excellent agreement between the two approaches. The findings of these researches were considered in the frame of complex systems theory, investigating how relationships between a system's parts can give rise to its collective behaviors and how the system interacts and forms relationships with its environment. In this view, the peculiar pharmacological behavior of biologically active natural compounds can be justified by the occurrence of molecular interactions due to the high complexity of the natural matrix. Some of these interactions have been widely studied in the case of green tea extracts (GTEs) proving unequivocally the presence of caffeine/catechin complexes in GTE samples. The presence of bimolecular complexes has been observed also in the case of Ceylon tea and Mate extracts. These data indicate that the formation of complexes in natural extracts is a common behavior and their presence must be considered in the description of natural extracts and, consequently, in their biological activity. ©2020 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2020-01-13
  • MASS SPECTROMETRY‐BASED PERSONALIZED DRUG THERAPY
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2020-01-05
    Jia‐Jia Cui; Lei‐Yun Wang; Zhi‐Rong Tan; Hong‐Hao Zhou; Xianquan Zhan; Ji‐Ye Yin

    Personalized drug therapy aims to provide tailored treatment for individual patient. Mass spectrometry (MS) is revolutionarily involved in this area because MS is a rapid, customizable, cost‐effective, and easy to be used high‐throughput method with high sensitivity, specificity, and accuracy. It is driving the formation of a new field, MS‐based personalized drug therapy, which currently mainly includes five subfields: therapeutic drug monitoring (TDM), pharmacogenomics (PGx), pharmacomicrobiomics, pharmacoepigenomics, and immunopeptidomics. Gas chromatography‐MS (GC‐MS) and liquid chromatography‐MS (LC‐MS) are considered as the gold standard for TDM, which can be used to optimize drug dosage. Matrix‐assisted laser desorption ionization‐time of flight‐MS (MALDI‐TOF‐MS) significantly improves the capability of detecting biomacromolecule, and largely promotes the application of MS in PGx. It is becoming an indispensable tool for genotyping, which is used to discover and validate genetic biomarkers. In addition, MALDI‐TOF‐MS also plays important roles in identity of human microbiome whose diversity can explain interindividual differences of drug response. Pharmacoepigenetics is to study the role of epigenetic factors in individualized drug treatment. MS can be used to discover and validate pharmacoepigenetic markers (DNA methylation, histone modification, and noncoding RNA). For the emerging cancer immunotherapy, personalized cancer vaccine has effective immunotherapeutic activity in the clinic. MS‐based immunopeptidomics can effectively discover and screen neoantigens. This article systematically reviewed MS‐based personalized drug therapy in the above mentioned five subfields. © 2020 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2020-01-06
  • THE USE OF MASS SPECTROMETRY TO STUDY ZN‐METALLOPROTEASE‐SUBSTRATE INTERACTIONS
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2020-01-03
    Giuseppe Grasso

    Zinc metalloproteases (ZnMPs) participate in diverse biological reactions, encompassing the synthesis and degradation of all the major metabolites in living organisms. In particular, ZnMPs have been recognized to play a very important role in controlling the concentration level of several peptides and/or proteins whose homeostasis has to be finely regulated for the correct physiology of cells. Dyshomeostasis of aggregation‐prone proteins causes pathological conditions and the development of several different diseases. For this reason, in recent years, many analytical approaches have been applied for studying the interaction between ZnMPs and their substrates and how environmental factors can affect enzyme activities. In this scenario, mass spectrometric methods occupy a very important role in elucidating different aspects of ZnMPs‐substrates interaction. These range from identification of cleavage sites to quantitation of kinetic parameters. In this work, an overview of all the main achievements regarding the application of mass spectrometric methods to investigating ZnMPs‐substrates interactions is presented. A general experimental protocol is also described which may prove useful to the study of similar interactions. © 2020 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2020-01-04
  • IDENTIFICATION OF MHC PEPTIDES USING MASS SPECTROMETRY FOR NEOANTIGEN DISCOVERY AND CANCER VACCINE DEVELOPMENT
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-12-25
    Rui Chen; Kelly M. Fulton; Susan M. Twine; Jianjun Li

    Immunotherapy with neoantigens presented by major histocompatibility complex (MHC) is one of the most promising approaches in cancer treatment. Using this approach, cancer vaccines can be designed to target tumor‐specific mutations that are not found in normal tissues. Clinical trials have demonstrated an increased immune response and eradication of tumors after injecting synthetic peptides selected from the immunopeptidome. Although the sequence of MHC binding peptides can be predicted from genome sequencing and prediction algorithms, this approach results in large numbers of predicted peptides, requiring the confirmation by mass spectrometry (MS) analysis. Identification of MHC peptides by direct MS analysis of immunopeptidome is accurate and sensitive, with tens of thousands of unique peptides potentially identified from either cancer cell line or tumor tissue. Peptides with mutations can also be identified with patient‐specific protein databases constructed from genome or transcriptome sequencing data. MS analysis also enables the characterization of the post‐translational modifications (PTMs) of those antigens that cannot be predicted. Moreover, PTMs were found to be more efficient in triggering an immune response. In addition to reviewing recent advances in the identification of neoantigens using MS, the techniques for cancer vaccine candidate selection and formulation, vaccine delivery systems, and the potential for use in combination with other therapeutics are also discussed. It is anticipated that MS‐based techniques will play an important role in future cancer vaccine development. © 2019 Wiley Periodicals, Inc. Mass Spec Rev 00:1–16, 2019.

    更新日期:2019-12-27
  • MASS SPECTROMETRY IN VIROLOGICAL SCIENCES
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-12-25
    Aleksandra Milewska; Joanna Ner‐Kluza; Agnieszka Dabrowska; Anna Bodzon‐Kulakowska; Krzysztof Pyrc; Piotr Suder

    Virology, as a branch of the life sciences, discovered mass spectrometry (MS) to be the pivotal tool around two decades ago. The technique unveiled the complex network of interactions between the living world of pro‐ and eukaryotes and viruses, which delivered “a piece of bad news wrapped in protein” as defined by Peter Medawar, Nobel Prize Laureate, in 1960. However, MS is constantly evolving, and novel approaches allow for a better understanding of interactions in this micro‐ and nanoworld. Currently, we can investigate the interplay between the virus and the cell by analyzing proteomes, interactomes, virus‐cell interactions, and search for the compounds that build viral structures. In addition, by using MS, it is possible to look at the cell from the broader perspective and determine the role of viral infection on the scale of the organism, for example, monitoring the crosstalk between infected tissues and the immune system. In such a way, MS became one of the major tools for the modern virology, allowing us to see the infection in the context of the whole cell or the organism. © 2019 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2019-12-27
  • THERAPEUTIC OLIGONUCLEOTIDES, IMPURITIES, DEGRADANTS, AND THEIR CHARACTERIZATION BY MASS SPECTROMETRY
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-12-16
    Soheil Pourshahian

    Oligonucleotides are an emerging class of drugs that are manufactured by solid‐phase synthesis. As a chemical class, they have unique product‐related impurities and degradants, characterization of which is an essential step in drug development. The synthesis cycle, impurities produced during the synthesis and degradation products are presented and discussed. The use of liquid chromatography combined with mass spectrometry for characterization and quantification of product‐related impurities and degradants is reviewed. In addition, sequence determination of oligonucleotides by gas‐phase fragmentation and indirect mass spectrometric methods is discussed. © 2019 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2019-12-17
  • MASS SPECTROMETRIC FRAGMENTATION OF TRIMETHYLSILYL AND RELATED ALKYLSILYL DERIVATIVES
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-12-05
    David J. Harvey, Paul Vouros

    This review describes the mass spectral fragmentation of trimethylsilyl (TMS) and related alkylsilyl derivatives used for preparing samples for analysis, mainly by combined gas chromatography and mass spectrometry (GC/MS). The review is divided into three sections. The first section is concerned with the TMS derivatives themselves and describes fragmentation of derivatized alcohols, thiols, amines, ketones, carboxylic acids and bifunctional compounds such as hydroxy‐ and amino‐acids, halo acids and hydroxy ethers. More complex compounds such as glycerides, sphingolipids, carbohydrates, organic phosphates, phosphonates, steroids, vitamin D, cannabinoids, and prostaglandins are discussed next. The second section describes intermolecular reactions of siliconium ions such as the TMS cation and the third section discusses other alkylsilyl derivatives. Among these latter compounds are di‐ and trialkyl‐silyl derivatives, various substituted‐alkyldimethylsilyl derivatives such as the tert‐butyldimethylsilyl ethers, cyclic silyl derivatives, alkoxysilyl derivatives, and 3‐pyridylmethyldimethylsilyl esters used for double bond location in fatty acid spectra. © 2019 Wiley Periodicals, Inc. Mass Spec Rev 0000:1–107, 2019

    更新日期:2019-12-06
  • MINIATURIZATION IN MASS SPECTROMETRY
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-12-03
    Przemyslaw Mielczarek, Jerzy Silberring, Marek Smoluch

    Expectations for continuous miniaturization in mass spectrometry are not declining for years. Portable instruments are highly welcome by the industry, science, space agencies, forensic laboratories, and many other units. All are striving for the small, cheap, and as good as possible instruments. This review describes the recent developments of miniature mass spectrometers and also provides selected applications where these devices are used. Upcoming perspectives of further development are also discussed. @ 2019 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2019-12-03
  • LABEL‐FREE BIO‐AFFINITY MASS SPECTROMETRY FOR SCREENING AND LOCATING BIOACTIVE MOLECULES
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-11-21
    Yi Tao, Jizhong Yan, Baochang Cai

    Despite the recent increase in the development of bioactive molecules in the drug industry, the enormous chemical space and lack of productivity are still important issues. Additional alternative approaches to screen and locate bioactive molecules are urgently needed. Label‐free bio‐affinity mass spectrometry (BA‐MS) provides opportunities for the discovery and development of innovative drugs. This review provides a comprehensive portrayal of BA‐MS techniques and of their applications in screening and locating bioactive molecules. After introducing the basic principles, alongside some application notes, the current state‐of‐the‐art of BA‐MS‐assisted drug discovery is discussed, including native MS, size‐exclusion chromatography‐MS, ultrafiltration‐MS, solid‐phase micro‐extraction‐MS, and cell membrane chromatography‐MS. Finally, several challenges and limitations of the current methods are summarized, with a view to potential future directions for BA‐MS‐assisted drug discovery. © 2019 Wiley Periodicals, Inc. Mass Spec Rev.

    更新日期:2019-11-22
  • MULTIOMIC patterns in body fluids: Technological challenge with a great potential to implement the advanced paradigm of 3P medicine
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-11-18
    Christopher Gerner, Vincenzo Costigliola, Olga Golubnitschaja

    Liquid biopsy (LB) is defined as a sample of any of body fluids (blood, saliva, tear fluid, urine, sweat, amniotic, cerebrospinal and pleural fluids, cervicovaginal secretion, and wound efflux, amongst others), which can be ex vivo analysed to detect and quantity the target(s) of interest. LB represents diagnostic approach relevant for organ‐specific changes and systemic health conditions including both manifested diseases and their prestages such as suboptimal health. Further, experts emphasise that DNA‐based analysis alone does not provide sufficient information for optimal diagnostics and effective treatments. Consequently, of great scientific and clinical utility are molecular patterns detected by hybrid technologies such as metabolomic tools and molecular imaging. Future proposed strategies utilise multiomic pillars (generally genome, tanscriptome, proteome, metabolome, epigenome, radiome, and microbiome), system‐biological approach, and multivariable algorithms for diagnostic, prognostic, and therapeutic purposes. Current article analyses pros and cons of the mass spectrometry‐based technologies, provides eminent examples of a success story “from discovery to clinical application,” and demonstrates a “road‐map” for the technology‐driven paradigm change from reactive to predictive, preventive and personalised medical services as the medicine of the future benefiting the patient and healthcare at large. © 2019 Wiley Periodicals, Inc. Mass Spec Rev

    更新日期:2019-11-18
  • The role of mass spectrometry and related techniques in the analysis of extractable and leachable chemicals
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-03-28
    Vincent P. Sica, Kady L. Krivos, Douglas E. Kiehl, Christopher J. Pulliam, Ian D. Henry, Timothy R. Baker

    In addition to degradation products, impurities, and exogenous contaminants, industries such as pharmaceutical, food, and others must concern themselves with leachables. These chemicals can derive from containers and closures or migrate from labels or secondary containers and packaging to make their way into products. Identification and quantification of extractables (potential leachables) and leachables, typically trace level analytes, is a regulatory expectation intended to ensure consumer safety and product fidelity. Mass spectrometry and related techniques have played a significant role in the analysis of extractables and leachables (E&L). This review provides an overview of how mass spectrometry is used for E&L studies, primarily in the context of the pharmaceutical industry. This review includes work flows, examples of how identification and quantification is done, and the importance of orthogonal data from several different detectors. E&L analyses are driven by the need for consumer safety. These studies are expected to expand in existing areas (e.g., food, textiles, toys, etc.) and into new, currently unregulated product areas. Thus, this topic is of interest to audiences beyond just the pharmaceutical and health care industries. Finally, the potential of universal detector approaches used in other areas is suggested as an opportunity to drive E&L research progress in this arguably understudied, under‐published realm.

    更新日期:2019-11-18
  • The Vouros Odyssey. Liquid chromatography/mass spectrometry from a chromatographic perspective and a Theseus Paradox
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2018-07-19
    Thomas Covey

    This article tracts Paul Vouro's contributions to the field of liquid chromatography ‐ mass spectrometry in the context of the history of the development of modern day LC/MS.

    更新日期:2019-11-18
  • The integration of LC‐MS and NMR for the analysis of low molecular weight trace analytes in complex matrices
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2018-07-19
    Rose M. Gathungu, Roger Kautz, Bruce S. Kristal, Susan S. Bird, Paul Vouros

    This review discusses the integration of liquid chromatography (LC), mass spectrometry (MS), and nuclear magnetic resonance (NMR) in the comprehensive analysis of small molecules from complex matrices. We first discuss the steps taken toward making the three technologies compatible, so as to create an efficient analytical platform. The development of online LC‐MS‐NMR, highlighted by successful applications in the profiling of highly concentrated analytes (LODs 10 μg) is discussed next. This is followed by a detailed overview of the alternative approaches that have been developed to overcome the challenges associated with online LC‐MS‐NMR that primarily stem from the inherently low sensitivity of NMR. These alternative approaches include the use of stop‐flow LC‐MS‐NMR, loop collection of LC peaks, LC‐MS‐SPE‐NMR, and offline NMR. The potential and limitations of all these approaches is discussed in the context of applications in various fields, including metabolomics and natural product discovery.

    更新日期:2019-11-18
  • DNA adducts: Formation, biological effects, and new biospecimens for mass spectrometric measurements in humans
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2018-06-11
    Byeong Hwa Yun, Jingshu Guo, Medjda Bellamri, Robert J. Turesky

    Hazardous chemicals in the environment and diet or their electrophilic metabolites can form adducts with genomic DNA, which can lead to mutations and the initiation of cancer. In addition, reactive intermediates can be generated in the body through oxidative stress and damage the genome. The identification and measurement of DNA adducts are required for understanding exposure and the causal role of a genotoxic chemical in cancer risk. Over the past three decades, 32P‐postlabeling, immunoassays, gas chromatography/mass spectrometry, and liquid chromatography/mass spectrometry (LC/MS) methods have been established to assess exposures to chemicals through measurements of DNA adducts. It is now possible to measure some DNA adducts in human biopsy samples, by LC/MS, with as little as several milligrams of tissue. In this review article, we highlight the formation and biological effects of DNA adducts, and highlight our advances in human biomonitoring by mass spectrometric analysis of formalin‐fixed paraffin‐embedded tissues, untapped biospecimens for carcinogen DNA adduct biomarker research.

    更新日期:2019-11-18
  • The expanding role of mass spectrometry in the field of vaccine development
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2018-05-31
    Vaneet Kumar Sharma, Ity Sharma, James Glick

    Biological mass spectrometry has evolved as a core analytical technology in the last decade mainly because of its unparalleled ability to perform qualitative as well as quantitative profiling of enormously complex biological samples with high mass accuracy, sensitivity, selectivity and specificity. Mass spectrometry‐based techniques are also routinely used to assess glycosylation and other post‐translational modifications, disulfide bond linkage, and scrambling as well as for the detection of host cell protein contaminants in the field of biopharmaceuticals. The role of mass spectrometry in vaccine development has been very limited but is now expanding as the landscape of global vaccine development is shifting towards the development of recombinant vaccines. In this review, the role of mass spectrometry in vaccine development is presented, some of the ongoing efforts to develop vaccines for diseases with global unmet medical need are discussed and the regulatory challenges of implementing mass spectrometry techniques in a quality control laboratory setting are highlighted.

    更新日期:2019-11-18
  • Anatomy and evolution of database search engines—a central component of mass spectrometry based proteomic workflows
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2017-09-13
    Kenneth Verheggen, Helge Ræder, Frode S. Berven, Lennart Martens, Harald Barsnes, Marc Vaudel

    Sequence database search engines are bioinformatics algorithms that identify peptides from tandem mass spectra using a reference protein sequence database. Two decades of development, notably driven by advances in mass spectrometry, have provided scientists with more than 30 published search engines, each with its own properties. In this review, we present the common paradigm behind the different implementations, and its limitations for modern mass spectrometry datasets. We also detail how the search engines attempt to alleviate these limitations, and provide an overview of the different software frameworks available to the researcher. Finally, we highlight alternative approaches for the identification of proteomic mass spectrometry datasets, either as a replacement for, or as a complement to, sequence database search engines.

    更新日期:2019-11-18
  • The Skyline ecosystem: Informatics for quantitative mass spectrometry proteomics
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2017-07-09
    Lindsay K. Pino, Brian C. Searle, James G. Bollinger, Brook Nunn, Brendan MacLean, Michael J. MacCoss

    Skyline is a freely available, open‐source Windows client application for accelerating targeted proteomics experimentation, with an emphasis on the proteomics and mass spectrometry community as users and as contributors. This review covers the informatics encompassed by the Skyline ecosystem, from computationally assisted targeted mass spectrometry method development, to raw acquisition file data processing, and quantitative analysis and results sharing.

    更新日期:2019-11-18
  • FUNCTIONAL METABOLOMICS DECIPHER BIOCHEMICAL FUNCTIONS AND ASSOCIATED MECHANISMS UNDERLIE SMALL‐MOLECULE METABOLISM
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2019-11-04
    Longlong Hu, Jingjing Liu, Wenhua Zhang, Tianyu Wang, Ning Zhang, Yie Hou Lee, Haitao Lu

    Metabolism is the collection of biochemical reactions enabled by chemically diverse metabolites, which facilitate different physiological processes to exchange substances and synthesize energy in diverse living organisms. Metabolomics has emerged as a cutting‐edge method to qualify and quantify the metabolites in different biological matrixes, and it has the extraordinary capacity to interrogate the biological significance that underlies metabolic modification and modulation. Liquid chromatography combined with mass spectrometry (LC/MS), as a robust platform for metabolomics analysis, has increased in popularity over the past 10 years due to its excellent sensitivity, throughput, and versatility. However, metabolomics investigation currently provides us with only phenotype data without revealing the biochemical functions and associated mechanisms. This limitation indeed weakens the core value of metabolomics data in a broad spectrum of the life sciences. In recent years, the scientific community has actively explored the functional features of metabolomics and translated this cutting‐edge approach to be used to solve key multifaceted questions, such as disease pathogenesis, the therapeutic discovery of drugs, nutritional issues, agricultural problems, environmental toxicology, and microbial evolution. Here, we are the first to briefly review the history and applicable progression of LC/MS‐based metabolomics, with an emphasis on the applications of metabolic phenotyping. Furthermore, we specifically highlight the next era of LC/MS‐based metabolomics to target functional metabolomes, through which we can answer phenotype‐related questions to elucidate biochemical functions and associated mechanisms implicated in dysregulated metabolism. Finally, we propose many strategies to enhance the research capacity of functional metabolomics by enabling the combination of contemporary omics technologies and cutting‐edge biochemical techniques. The main purpose of this review is to improve the understanding of LC/MS‐based metabolomics, extending beyond the conventional metabolic phenotype toward biochemical functions and associated mechanisms, to enhance research capability and to enlarge the applicable scope of functional metabolomics in small‐molecule metabolism in different living organisms.

    更新日期:2019-11-04
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  • MENTOR, COLLABORATOR, AND FRIEND.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : null
    Ivan C Gerling

    更新日期:2019-11-01
  • Lessons in de novo peptide sequencing by tandem mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2015-02-11
    Katalin F Medzihradszky,Robert J Chalkley

    Mass spectrometry has become the method of choice for the qualitative and quantitative characterization of protein mixtures isolated from all kinds of living organisms. The raw data in these studies are MS/MS spectra, usually of peptides produced by proteolytic digestion of a protein. These spectra are "translated" into peptide sequences, normally with the help of various search engines. Data acquisition and interpretation have both been automated, and most researchers look only at the summary of the identifications without ever viewing the underlying raw data used for assignments. Automated analysis of data is essential due to the volume produced. However, being familiar with the finer intricacies of peptide fragmentation processes, and experiencing the difficulties of manual data interpretation allow a researcher to be able to more critically evaluate key results, particularly because there are many known rules of peptide fragmentation that are not incorporated into search engine scoring. Since the most commonly used MS/MS activation method is collision-induced dissociation (CID), in this article we present a brief review of the history of peptide CID analysis. Next, we provide a detailed tutorial on how to determine peptide sequences from CID data. Although the focus of the tutorial is de novo sequencing, the lessons learned and resources supplied are useful for data interpretation in general.

    更新日期:2019-11-01
  • Protein modifications by electrophilic lipoxidation products: adduct formation, chemical strategies and tandem mass spectrometry for their detection and identification.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2014-05-13
    Yury V Vasil'ev,Shin-Chen Tzeng,Lin Huang,Claudia S Maier

    The post-translational modification of proteins by electrophilic oxylipids is emerging as an important mechanism that contributes to the complexity of proteomes. Enzymatic and non-enzymatic oxidation of biological lipids results in the formation of chemically diverse electrophilic carbonyl compounds, such as 2-alkenals and 4-hydroxy alkenals, epoxides, and eicosanoids with reactive cyclopentenone structures. These lipoxidation products are capable of modifying proteins. Originally considered solely as markers of oxidative insult, more recently the modifications of proteins by lipid peroxidation products are being recognized as a new mechanism of cell signaling with relevance to redox homeostasis, adaptive response and inflammatory resolution. The growing interest in protein modifications by reactive oxylipid species necessitates the availability of methods that are capable of detecting, identifying and characterizing these protein adducts in biological samples with high complexity. However, the efficient analysis of these chemically diverse protein adducts presents a considerable analytical challenge. We first provide an introduction into the chemistry and biological relevance of protein adductions by electrophilic lipoxidation products. We then provide an overview of tandem mass spectrometry approaches that have been developed in recent years for the interrogation of protein modifications by electrophilic oxylipid species.

    更新日期:2019-11-01
  • Gas phase basicities of polyfunctional molecules. Part 3: Amino acids.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2012-05-23
    Guy Bouchoux

    The present article is the third part of a general overview of the gas-phase protonation thermochemistry of polyfunctional molecules (first part: Mass Spectrom. Rev., 2007, 26:775-835, second part: Mass Spectrom. Rev., 2011, in press). This review is devoted to the 20 proteinogenic amino acids and is divided in two parts. In the first one, the experimental data obtained during the last 30 years using the equilibrium, thermokinetic and kinetic methods are presented. A general re-assignment of the values originating from these various experiments has been done on the basis of the commonly accepted Hunter & Lias 1998 gas-phase basicity scale in order to provide an homogeneous set of data. In the second part, theoretical investigations on gaseous neutral and protonated amino acids are reviewed. Conformational landscapes of both types of species were examined in order to provide theoretical protonation thermochemistry based on the truly identified most stable conformers. Proton affinities computed at the presently highest levels of theory (i.e. composite methods such as Gn procedures) are presented. Estimates of thermochemical parameters calculated using a Boltzmann distribution of conformers at 298K are also included. Finally, comparison between experiment and theory is discussed and a set of evaluated proton affinities, gas-phase basicities and protonation entropies is proposed.

    更新日期:2019-11-01
  • Preface to the special issue of Mass Spectrometry Reviews.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2018-10-23
    Dietmar Kuck,Jürgen Grotemeyer

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  • James Augustus McCloskey (1936-2017).
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2018-02-08
    Paul Vouros,Dominic Desiderio

    更新日期:2019-11-01
  • Determination of dioxins/furans and PCBs by quadrupole ion-trap gas chromatography-mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-11-18
    J B Plomley,M Lausevic,R E March

    The versatility and sensitivity of the quadrupole ion trap tandem mass spectrometer has been applied to the determination of polychlorodibenzo-p-dioxins (PCDDs) and polychlorodibenzofurans (PCDFs), and of polychlorinated biphenyls (PCBs). A brief introduction to the theory of ion confinement in a quadrupole ion trap permits discussion of ion trajectory stability, mass-selective ion ejection, the frequencies of ion motion, and the role of resonant excitation of ion motion. The tandem mass spectrometric examination of PCDDs and PCDFs eluting and co-eluting from a gas chromatographic column is described. Illustrative examples are given of the analysis of field samples containing PCDDs and PCDFs. A comparison is presented of the performance of each of a quadrupole ion trap tandem mass spectrometer, a triple stage quadrupole mass spectrometer, and a sector instrument of relatively high mass resolution for the determination of PCDDs and PCDFs. This comparison is made with respect to instrument tuning, calibration plots, detection limits, ion signals at low concentration, relative response factors, ionization cross-sections, and the examination of field samples. The application of quadrupole ion trap tandem mass spectrometry to the examination of PCBs is focused upon those PCB congeners that have the greatest toxicity. 39 congeners of the total of 209 PCB congeners have been identified as having the greatest toxicities. Chemical ionization has been used for the determination of co-eluting congeners #77 and #110 where the toxicity of the former is much greater than that of the latter. An analytical protocol, based on the variation of molecular ion fragmentation according to the degree (or absence) of chlorine ortho-substitution, has been proposed for distinguishing between toxic and nontoxic PCB congeners.

    更新日期:2019-11-01
  • The role of mass spectrometry in the study of non-enzymatic protein glycation in diabetes.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-11-18
    A Lapolla,D Fedele,P Traldi

    Mass spectrometry has been applied successfully to the study of non-enzymatic protein glycation, which is a topic of wide interest in the diabetes field. Low- and high-resolution mass spectra, GC/MS, and collisional activation spectroscopy allow the structural identification and quantitative evaluation of advanced glycation end-products, which represent important molecules for monitoring diabetes. More recently available techniques, such as ESI and MALDI/MS, have had a significant impact on analytical problems in diabetes. In particular, MALDI has been applied to the study of protein glycation in in vitro and in vivo conditions, because the number of glucose molecules that condense onto the protein can be easily determined by this approach. In the former case, glycation kinetics have been studied in various sugars and sugar concentrations, proteins, and buffer concentrations; in the latter, comparisons of MALDI spectra of circulating proteins from healthy and diabetic subjects determine the exposure of patients to high glucose levels. The method has been applied to an evaluation of the glycation level of immunoglobulins, and indicates that glycation takes place preferentially on the Fab fragment of the protein; data are relevant in relating immunological impairment with glycation-induced changes in the functionality of immunoglobulins.

    更新日期:2019-11-01
  • Real-time single particle mass spectrometry: a historical review of a quarter century of the chemical analysis of aerosols
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-09-15
    Noble,Prather

    Real-time single particle mass spectrometry, or continuous aerosol mass spectrometry, was originally developed in the 1970s for the purpose of identifying the chemical composition of airborne particulate matter in real-time. Although this technique has continued to evolve throughout the following decades, the fundamental characteristic of this method remains the same, involving the continuous introduction of solid particle or liquid droplets directly into the ion source region of a mass spectrometer. Continuous sample introduction allows for the chemical analysis of single airborne particles in real-time. A number of mass analyzers have been employed in real-time single particle mass spectrometry. The original real-time single particle mass spectrometer used a magnetic sector mass analyzer. Quadrupole, double-focusing, and ion trap mass spectrometers have also been utilized. The majority of the current real-time single particle mass spectrometry techniques use time-of-flight mass spectrometry. In the literature, a variety of general names have been applied to real-time single particle mass spectrometry methods. These names include direct-inlet mass spectrometry, on-line laser microprobe mass spectrometry, particle analysis by mass spectrometry, particle beam mass spectrometry, and rapid-single particle mass spectrometry. This review covers real-time single particle mass spectrometry techniques that were developed from 1973 through 1998, specifically for analyzing airborne particulate matter, including environmental aerosols, biological aerosols, and clean-room aerosols. Because the majority of the historical and current real-time single particle mass spectrometers have been employed for atmospheric aerosols, this topic is the primary focus of this review. This review does not include on-line mass spectrometry methods that are employed as a detector for other instrumental methods, such as liquid chromatography.

    更新日期:2019-11-01
  • Noncovalent metal-ligand bond energies as studied by threshold collision-induced dissociation
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-09-15
    Rodgers,Armentrout

    This review focuses on noncovalent metal ion-ligand complexes and measurements of the bond energies of such species. The method utilized in this work is threshold collision-induced dissociation (CID), as achieved using a guided ion beam tandem mass spectrometer. Accurate determination of bond energies requires attention to many details of the experiments and data analysis. These details are discussed thoroughly and compared to other methods. A comprehensive listing of metal-ligand bond dissociation energies determined by threshold CID is provided. This list includes a variety of metals (alkalis, magnesium, aluminum, and first and second row transition metals), many different types of ligands, and variations in the number of ligands. The trends in these values are discussed, and we elucidate the importance of ion-dipole and ion-induced dipole interactions, chelation, different conformers and tautomers, steric interactions, solvation phenomena, and electronic effects such as hybridization and promotion.

    更新日期:2019-11-01
  • Liquid chromatography-mass spectrometry in forensic toxicology.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-09-15
    J F Van Bocxlaer,K M Clauwaert,W E Lambert,D L Deforce,E G Van den Eeckhout,A P De Leenheer

    Liquid chromatography-mass spectrometry has evolved from a topic of mainly research interest into a routinely usable tool in various application fields. With the advent of new ionization approaches, especially atmospheric pressure, the technique has established itself firmly in many areas of research. Although many applications prove that LC-MS is a valuable complementary analytical tool to GC-MS and has the potential to largely extend the application field of mass spectrometry to hitherto "MS-phobic" molecules, we must recognize that the use of LC-MS in forensic toxicology remains relatively rare. This rarity is all the more surprising because forensic toxicologists find themselves often confronted with the daunting task of actually searching for evidence materials on a scientific basis without any indication of the direction in which to search. Through the years, mass spectrometry, mainly in the GC-MS form, has gained a leading role in the way such quandaries are tackled. The advent of robust, bioanalytically compatible combinations of liquid chromatographic separation with mass spectrometric detection really opens new perspectives in terms of mass spectrometric identification of difficult molecules (e.g., polar metabolites) or biopolymers with toxicological relevance, high throughput, and versatility. Of course, analytical toxicologists are generally mass spectrometry users rather than mass spectrometrists, and this difference certainly explains the slow start of LC-MS in this field. Nevertheless, some valuable applications have been published, and it seems that the introduction of the more universal atmospheric pressure ionization interfaces really has boosted interests. This review presents an overview of what has been realized in forensic toxicological LC-MS. After a short introduction into LC-MS interfacing operational characteristics (or limitations), it covers applications that range from illicit drugs to often abused prescription medicines and some natural poisons. As such, we hope it can act as an appetizer to those involved in forensic toxicology but still hesitating to invest in LC-MS.

    更新日期:2019-11-01
  • Mass spectrometry in combinatorial chemistry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-07-21
    C Enjalbal,J Martinez,J L Aubagnac

    In the fast expanding field of combinatorial chemistry, profiling libraries has always been a matter of concern--as illustrated by the buoyant literature over the past seven years. Spectroscopic methods, including especially mass spectrometry and to a lesser extent IR and NMR, have been applied at different levels of combinatorial library synthesis: in the rehearsal phase to optimize the chemistry prior to library generation, to confirm library composition, and to characterize after screening each structure that exhibits positive response. Most of the efforts have been concentrated on library composition assessment. The difficulties of such analyses have evolved from the infancy of the combinatorial concept, where large mixtures were prepared, to the recent parallel syntheses of collections of discrete compounds. Whereas the complexity of the analyses has diminished, an increased degree of automation was simultaneously required to achieve efficient library component identification and quantification. In this respect, mass spectrometry has been found to be the method of choice, providing rapid, sensitive, and informative analyses, especially when coupled to chromatographic separation. Fully automated workstations able to cope with several hundreds of compounds per day have been designed. After a brief introduction to describe the combinatorial approach, library characterization will be discussed in detail, considering first the solution-based methodologies and secondly the support-bound material analyses.

    更新日期:2019-11-01
  • Alkali-metal ion/molecule association reactions and their applications to mass spectrometry
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-07-21
    Fujii

    This review will be concerned primarily with thermal alkali-metal ion association reactions of the general type: A+ + M + N reversible (A + M)+ + N. Where A denotes a positively charged alkali metal ion, M is neutral species and N works as a third body. As indicated, most association reactions are reversible, and the A-M bond derives primarily from electrostatic forces whose energy (affinity) is typically 50 kcal/mol or less, often much less. The review includes reaction mechanism, instrumentation, and application to mass spectrometry, together with reaction rates and alkali ion affinities of the classified compounds.

    更新日期:2019-11-01
  • Orthogonal acceleration time-of-flight mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-05-05
    M Guilhaus,D Selby,V Mlynski

    The principles and applications of time-of-flight mass spectrometry involving instruments with independent (orthogonal) axes for ion generation and mass analysis are reviewed. This approach, generally referred to as orthogonal acceleration time-of-flight mass spectrometry, has proved particularly advantageous for the combination of continuous ionization sources with time-of-flight mass spectrometry. The history of the technique is briefly discussed along with the instrumental principles pertaining to all the stages of the instrumentation from ion source to detector. The applications of commercial and customized instruments are discussed for several ionization methods including electrospray, matrix assisted laser desorption/ionization, electron ionization, and plasma ionization.

    更新日期:2019-11-01
  • Membrane introduction mass spectrometry: trends and applications.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-03-15
    R C Johnson,R G Cooks,T M Allen,M E Cisper,P H Hemberger

    Recent advances in membrane introduction mass spectrometry (MIMS) are reviewed. On-line monitoring is treated by focusing on critical variables, including the nature and dimensions of the membrane, and the analyte vapor pressure, diffusivity, and solubility in the membrane barrier. Sample introduction by MIMS is applied in (i) on-line monitoring of chemical and biological reactors, (ii) analysis of volatile organic compounds in environmental matrices, including air, water and soil, and (iii) in more fundamental studies, such as measurements of thermochemical properties, reaction mechanisms, and kinetics. New semipermeable membranes are discussed, including those consisting of thin polymers, low vapor pressure liquids, and zeolites. These membranes have been used to monitor polar compounds, selectively differentiate compounds through affinity-binding, and provide isomer differentiation based on molecular size. Measurements at high spatial resolution, for example, using silicone-capped hypodermic needle inlets, are also covered, as is electrically driven sampling through microporous membranes. Other variations on the basic MIMS experiment include analyte preconcentration through cryotrapping (CT-MIMS) or trapping in the membrane (trap-and-release), as well as differential thermal release methods and reverse phase (i.e., organic solvent) MIMS. Method limitations center on semivolatile compounds and complex mixture analysis, and novel solutions are discussed. Semivolatile compounds have been monitored with thermally assisted desorption, ultrathin membranes and derivatization techniques. Taking advantage of the differences in time of membrane permeation, mixtures of structurally similar compounds have been differentiated by using sample modulation techniques and by temperature-programmed desorption from a membrane interface. Selective ionization techniques that increase instrument sensitivity towards polar compounds are also described, and comparisons are made with other direct sampling (nonchromatographic) methods that are useful in mixture analysis.

    更新日期:2019-11-01
  • Contributions of C3H6O+. ions with the oxygen on the middle carbon to gas phase ion chemistry
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-03-15
    McAdoo

    The numerous ways in which studies of C3H6O+. ions with the oxygen on the second carbon have added to our knowledge of gas phase ion chemistry are reviewed. The enol form of this ion (1) first attracted interest during early investigations of the mechanism of the McLafferty Rearrangement and later in characterizing the double McLafferty Rearrangement. Next, it was found that 1 isomerizes to the higher energy acetone ion (2). This discovery sparked studies of the relative stabilities of ionized and neutral enol and ketone species. It also led to the discovery that 1-->2 surmounts a substantial barrier, and that 2 dissociates faster than the excess energy deposited in it by the isomerization can become randomly distributed; i.e., dissociation following 1-->2 is nonergodic. This fact is manifested by a more abundant loss of the methyl formed by isomerization and a greater associated translational energy release. Propene oxide and methyl vinyl ether ions also appear to ionize to 2 and to dissociate nonergodically. Methane is eliminated from 2 through a methyl-acetyl ion complex. Characterization of this reaction by photoionization mass spectrometry, ab initio theory, and RRKM calculations helped to establish that complex-mediated alkane eliminations are generally confined to a region just above threshold. At higher energies, because attractions between ions and nonpolar neutrals are weak, simple dissociation is too fast for complex-mediated H-transfer to compete with it. Studies of the collision-induced dissociations of 2 demonstrate that the first electronically excited A state of 2 is very long-lived and efficiently releases its energy into translational energy when the ion collides with a neutral at low impact energies. Finally, ion-molecule reactions of 2 and acetone-containing ion clusters in the gas phase are described.

    更新日期:2019-11-01
  • Matrix-assisted laser desorption/ionization mass spectrometry of carbohydrates.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2000-01-19
    D J Harvey

    This review describes the application of matrix-assisted laser desorption/ionization (MALDI) mass spectrometry to carbohydrate analysis and covers the period 1991-1998. The technique is particularly valuable for carbohydrates because it enables underivatised, as well as derivatised compounds to be examined. The various MALDI matrices that have been used for carbohydrate analysis are described, and the use of derivatization for improving mass spectral detection limits is also discussed. Methods for sample preparation and for extracting carbohydrates from biological media prior to mass spectrometric analysis are compared with emphasis on highly sensitive mass spectrometric methods. Quantitative aspects of MALDI are covered with respect to the relationship between signal strength and both mass and compound structure. The value of mass measurements by MALDI to provide a carbohydrate composition is stressed, together with the ability of the technique to provide fragmentation spectra. The use of in-source and post-source decay and collision-induced fragmentation in this context is described with emphasis on ions that provide information on the linkage and branching patterns of carbohydrates. The use of MALDI mass spectrometry, linked with exoglycosidase sequencing, is described for N-linked glycans derived from glycoproteins, and methods for the analysis of O-linked glycans are also covered. The review ends with a description of various applications of the technique to carbohydrates found as constituents of glycoproteins, bacterial glycolipids, sphingolipids, and glycolipid anchors.

    更新日期:2019-11-01
  • LC/MS applications in drug development.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-11-24
    M S Lee,E H Kerns

    The combination of high-performance liquid chromatography and mass spectrometry (LC/MS) has had a significant impact on drug development over the past decade. Continual improvements in LC/MS interface technologies combined with powerful features for structure analysis, qualitative and quantitative, have resulted in a widened scope of application. These improvements coincided with breakthroughs in combinatorial chemistry, molecular biology, and an overall industry trend of accelerated development. New technologies have created a situation where the rate of sample generation far exceeds the rate of sample analysis. As a result, new paradigms for the analysis of drugs and related substances have been developed. The growth in LC/MS applications has been extensive, with retention time and molecular weight emerging as essential analytical features from drug target to product. LC/MS-based methodologies that involve automation, predictive or surrogate models, and open access systems have become a permanent fixture in the drug development landscape. An iterative cycle of "what is it?" and "how much is there?" continues to fuel the tremendous growth of LC/MS in the pharmaceutical industry. During this time, LC/MS has become widely accepted as an integral part of the drug development process. This review describes the utility of LC/MS techniques for accelerated drug development and provides a perspective on the significant changes in strategies for pharmaceutical analysis. Future applications of LC/MS technologies for accelerated drug development and emerging industry trends are also discussed.

    更新日期:2019-11-01
  • Energy-sensitive cryogenic detectors for high-mass biomolecule mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-11-24
    M Frank,S E Labov,G Westmacott,W H Benner

    Energy-sensitive calorimetric detectors that operate at low temperatures ("cryogenic detectors") have recently been applied for the first time as ion detectors in time-of-flight mass spectrometry. Compared to conventional, ionization-based detectors, which rely on secondary electron formation or the charge created in a semiconductor, cryogenic detectors measure low-energy solid state excitations created by a particle impact. This energy sensitivity of cryogenic detectors results in several potential advantages for TOF-MS. Cryogenic detectors are expected to have near 100% efficiency even for very large, slow-moving molecules, in contrast to microchannel plates whose efficiency drops considerably at large mass. Thus, cryogenic detectors could contribute to extending the mass range accessible by TOF-MS and help improving detection limits. In addition, the energy resolution provided by cryogenic detectors can be used for charge discrimination and studies of ion fragmentation, ion-detector interaction, and internal energies of large molecular ions. Cryogenic detectors could therefore prove to be a valuable diagnostic tool in TOF-MS. Here, we give a general introduction to the cryogenic detector types most applicable to TOF-MS including those types already used in several TOF-MS experiments. We review and compare the results of these experiments, discuss practical aspects of operating cryogenic detectors in TOF-MS systems, and describe potential near future improvements of cryogenic detectors for applications in mass spectrometry.

    更新日期:2019-11-01
  • The role of liquid chromatography-mass spectrometry in the determination of heroin and related opioids in biological fluids.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-10-12
    S Pichini,I Altieri,M Pellegrini,P Zuccaro,R Pacifici

    The opioid most commonly sold in the illicit market is heroin. This substance, classified as an analgesic narcotic drug, has an extremely short half-life, and it is rapidly metabolized to 6-monoacetyl-morphine and further to morphine. Morphine is principally metabolized by conjugation to morphine-3 and morphine-6 glucuronides. Morphine itself is a potent analgesic that is frequently used in the pharmacological intervention of cancer pain. The toxicological and clinical evaluation of heroin and morphine have stimulated pharmacokinetic studies in human and animal models. Although a number of methods exist to determine opiates and their metabolites, liquid chromatography (LC) appears to be the technique that can separate without any pretreatment the lipophilic and the hydrophilic analytes of the complete metabolic profile of heroin and/or morphine. Moreover, mass spectrometry (MS) used as a detector for liquid chromatography is unique, because it offers universality and selectivity. Furthermore, efforts have been made to develop LC/MS interfaces that could overcome the previous problem of poor sensitivity. For this reason, in recent years LC combined with MS has been applied to the analysis of opiates--parent drugs and metabolites--in biological fluids. This article reviews the existing literature on the determination, using liquid chromatography coupled to mass spectrometry, of opiate metabolites found in different biological matrices after the administration of the parent compounds.

    更新日期:2019-11-01
  • Ion/ion chemistry of high-mass multiply charged ions.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-06-09
    S A McLuckey,J L Stephenson

    Electrospray ionization has enabled the establishment of a new area of ion chemistry research based on the study of the reactions of high-mass multiply charged ions with ions of opposite polarity. The multiple-charging phenomenon associated with electrospray makes possible the generation of multiply charged reactant ions that yield charged products as a result of partial neutralization due to ion/ion chemistry. The charged products can be readily studied with mass spectrometric methods, providing useful insights into reaction mechanisms. This review presents the research done in this area, all of which has been performed within the past decade. Ion/ion chemistry has been studied at near-atmospheric pressure in a reaction region that leads to the atmospheric/vacuum interface of a mass spectrometer, and within a quadrupole ion trap operated with a bath gas at a pressure of 1 mtorr. Proton transfer has been the most common reaction type for high-mass ions, but other forms of "charge transfer," such as electron transfer and fluoride transfer, have also been observed. For some ion/ion reactions, attachment of the two reactants has been observed. Multiply charged ion/ion reactions are fast, due to the long-range Coulombic attraction, and they are universal in that any pair of oppositely charged ions is expected to react due to the high exothermicity associated with mutual neutralization. The kinetics of reaction for multiply charged ions, derived from the same molecule with a given singly charged reactant ion, follow a charge-squared dependence, at least under normal quadrupole ion trap conditions. This dependence suggests that reaction rates are determined by the long-range Coulomb attraction, and that the ions react with constant efficiency as a function of charge state. In the case of proton transfer reactions from polypeptides to even-electron perfluorocarbon anions, no fragmentation of the polypeptide product ions has, as yet, been observed. Electron transfer from small oligonucleotide anions to rare gas cations, on the other hand, results in extensive fragmentation of the nucleic acid product ions. The extent of fragmentation decreases as the size of the oligonucleotide anions increases, reflecting a decrease in fragmentation rates associated with an increase in the number of internal degrees of freedom of the oligonucleotide. When ion-cooling rates become competitive with dissociation rates, the initially formed product ions are stabilized and fragmentation is avoided. Collisional cooling, therefore, likely plays an important role in the relative lack of dissociation observed thus far as a result of ion/ion reactions for most high-mass ions. The observed dependence of ion/ion reaction rates on the square of the ion charge, the universal nature of mutual neutralization, and the relative lack of fragmentation that arises from ion/ion reactions, makes ion/ion chemistry a particularly useful means for manipulating charge states. This review emphasizes applications that take advantage of the unique characteristics of ion/ion proton transfer chemistry for manipulating charge states. These applications include mixture analysis by electrospray, precursor ion charge state manipulation for tandem mass spectrometry studies, and simplified interpretation of product ion spectra.

    更新日期:2019-11-01
  • Contribution of mass spectrometry to contemporary immunology.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-05-13
    A de Jong

    Mass spectrometry has become an increasingly important tool in the characterization of histocompatibility complex molecule (MHC) bound antigen peptides. It is one of the few technologies capable of identifying minute amounts of peptides in complex (5,000-10,000 constituents) MHC elution mixtures. Currently, the combination of tandem mass spectrometry with electrospray ionization (ESI) and microcapillary liquid chromatography (microLC) has proven to be the more versatile and effective technology. Post-source decay (PSD) and on-slide digestion combined with matrix-assisted laser desorption/ionization time-of-flight (MALDI-ToF) may be valuable as well in certain circumstances. Recent refinements in the technology, such as the development of the quadrupole ion trap (QIT), Fourier transform ion cyclotron resonance (FTICR), and orthogonal quadrupole-time-of-flight (qToF) mass spectrometers equipped with nanoscale electrospray ionization sources and combined with microscale LC or capillary zone electrophoresis (CZE) yield attomole-range sensitivity in peptide sequencing, a level approaching the immuno-relevant level to a significant extent. In this review, past and ongoing developments in mass spectrometry and analytical separation techniques and their application to contemporary immunology are discussed.

    更新日期:2019-11-01
  • Charge derivatization of peptides for analysis by mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-05-04
    K D Roth,Z H Huang,N Sadagopan,J T Watson

    The analysis of peptide derivatives by fast atom bombardment, liquid secondary-ionization mass spectrometry, plasma desorption, electrospray ionization, and matrix-assisted laser desorption/ionization is reviewed. The fragmentation patterns of peptides and of charge-derivatized peptides are compared, and the proposed fragment ion structures are summarized. A variety of derivatization approaches and the distinguishing features of mass spectra produced from these derivatives are described. The most promising derivatization approaches are evaluated, and the strengths and limitations of these approaches are discussed.

    更新日期:2019-11-01
  • Urinary nucleosides.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-03-30
    K H Schram

    The methods of analysis, origins, and clinical significance of urinary nucleosides are reviewed through 1997. Structures, chromatographic and mass spectral data and references to the clinical literature are presented for each of the 57 nucleosides currently identified in normal and pathogenic human urine samples. Data from the HPLC separation and GC/MS analysis of 37 individual HPLC fractions are presented and discussed. Methods, including sample preparation techniques, used for the analysis of urinary nucleosides including GC, HPLC, GC/MS, HPLC/MS and immunoassays are compared and the advantages and limitations of each method described. The conclusion is drawn that the urinary nucleosides do serve as biomarkers of cancer and other diseases, but analytical methods need further improvement if clinical decisions are to be made based on the levels of nucleosides in human urine.

    更新日期:2019-11-01
  • Mass spectrometric analysis of lipo-chitin oligosaccharides--signal molecules mediating the host-specific legume-rhizobium symbiosis.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1999-02-10
    K M van der Drift,M M Olsthoorn,L P Brüll,L Blok-Tip,J E Thomas-Oates

    Lipo-chitin oligosaccharides (LCOs) are novel bacterial glycolipid signal molecules that mediate the species--specific symbiosis between rhizobial bacteria and leguminous plants. Nodulation of the legume roots and nitrogen-fixation in the resulting nodules by Rhizobia is controlled by the bacterial nodulation genes that encode the LCO biosynthetic enzymes. The length of the LCO chitin backbone, the length and degree of unsaturation of the fatty acyl chain attached to it, and the combination of different chemical substituents on the reducing- and nonreducing-terminal residues all contribute to the species--specificity of the signal. LCOs are bioactive in the nanomolar and subnanomolar concentration range and are produced as heterogeneous mixtures, making determination of their structures a difficult task, most successfully approached by the application of modern mass spectrometric methods in combination with specific chemical treatments aimed at identifying specific chemical moieties. This review presents an overview of these methods as they are being used for the structural elucidation of LCOs, and discusses the role of structural diversity in mediating species-specificity.

    更新日期:2019-11-01
  • Fourier transform ion cyclotron resonance mass spectrometry: a primer.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1998-10-13
    A G Marshall,C L Hendrickson,G S Jackson

    This review offers an introduction to the principles and generic applications of FT-ICR mass spectrometry, directed to readers with no prior experience with the technique. We are able to explain the fundamental FT-ICR phenomena from a simplified theoretical treatment of ion behavior in idealized magnetic and electric fields. The effects of trapping voltage, trap size and shape, and other nonidealities are manifested mainly as perturbations that preserve the idealized ion behavior modified by appropriate numerical correction factors. Topics include: effect of ion mass, charge, magnetic field, and trapping voltage on ion cyclotron frequency; excitation and detection of ICR signals; mass calibration; mass resolving power and mass accuracy; upper mass limit(s); dynamic range; detection limit, strategies for mass and energy selection for MSn; ion axialization, cooling, and remeasurement; and means for guiding externally formed ions into the ion trap. The relation of FT-ICR MS to other types of Fourier transform spectroscopy and to the Paul (quadrupole) ion trap is described. The article concludes with selected applications, an appendix listing accurate fundamental constants needed for ultrahigh-precision analysis, and an annotated list of selected reviews and primary source publications that describe in further detail various FT-ICR MS techniques and applications.

    更新日期:2019-11-01
  • The use of bioreactive probes in protein characterization.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1998-08-15
    R W Nelson

    Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF) has in the past decade found routine use in the biological sciences. With this use has evolved several mass spectrometric-based methods directed at the intricate investigation of biomolecular structure and function. One such methodology involves the enzymatic modification of a protein prior to the mass spectrometric readout of the resulting products. The enzyme-modification/mass spectrometric approach has a definite use in a number of applications, including: the verification/identification of protein sequence, elucidation of post-translational modifications, the investigation of protein higher-order structure, and even the characterization of the modifying enzyme. To avoid the potentials of sample loss and autolytic interferences in the mass spectrum, mass spectrometer targets can be covalently derivatized with enzymes for use in the characterization procedures. The enzymatically active, or bioreactive, probes are used by application of the analyte to the activated surface, followed by application of a suitable MALDI matrix and mass analysis from the surface of the probe. Limited transfer and handling steps eliminate sample losses, and surface-tethered enzymes (and autolytic fragments) are prohibited from interfering with analytical signals in the mass spectra. In addition, the probes are rapid and easy to use. Reviewed here are issues of concern during the manufacture and use of the bioreactive probes, and application of the probes to investigate protein structure and function.

    更新日期:2019-11-01
  • Mass spectrometry in the search for uremic toxins.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1998-08-15
    T Niwa

    This article reviews the literature on the mass spectrometry (MS) that has been used in the research of uremic toxins. Gas chromatography/mass spectrometry (GC/MS) has been most often used for the analysis of low-molecular-weight compounds in uremic blood such as organic acids, phenols, and polyols. However, it cannot be used for the analysis of middle- to high-molecular-weight substances or for involatile compounds. The development of fast atom bombardment (FAB) and liquid secondary ion mass spectrometry (LSIMS) has made possible the analysis of middle-molecules and involatile low-molecular-weight substances such as peptides and nucleosides. The development of atmospheric pressure chemical ionization (APCI) has also lead to the analysis of involatile low-molecular-weight substances. The recent advances in ionization methods, such as electrospray ionization (ESI) and matrix-assisted laser desorption ionization (MALDI), have permitted the MS analysis of high-molecular-weight substances such as beta 2-microglobulin, a major component of dialysis amyloid. Liquid chromatography/mass spectrometry (LC/MS), using ESI, APCI, or FAB as an ionization method, is currently the preferred method for the analysis of low- to high-molecular-weight substances in uremic blood. ESI-LC/MS and matrix-assisted laser desorption ionization-time of flight mass spectrometry (MALDI-TOFMS) are useful for elucidating the structure of post-translationally modified proteins obtained from the blood and tissues of uremic patients. Post-translational modification such as the formation of advanced glycation end-products and carbamoylation is enhanced in uremic patients, and is considered to be responsible for some uremic symptoms. Laser microprobe MS is unique in its capability for the two-dimensional detection of atoms such as aluminum in a tissue section obtained from uremic patients. This review focuses on the mainstream research for discovering uremic toxins, specific uremic toxins identified or quantified using MS, and the MS analysis of post-translationally modified proteins in uremia. These studies have provided ample evidence that MS has played an important role in the search for uremic toxins.

    更新日期:2019-11-01
  • High-precision continuous-flow isotope ratio mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1998-04-16
    J T Brenna,T N Corso,H J Tobias,R J Caimi

    Although high-precision isotope determinations are routine in many areas of natural science, the instrument principles for their measurements have remained remarkably unchanged for four decades. The introduction of continuous-flow techniques to isotope ratio mass spectrometry (IRMS) instrumentation has precipitated a rapid expansion in capabilities for high-precision measurement of C, N, O, S, and H isotopes in the 1990s. Elemental analyzers, based on the flash combustion of solid organic samples, are interfaced to IRMS to facilitate routine C and N isotopic analysis of unprocessed samples. Gas/liquid equilibrators have automated O and H isotopic analysis of water in untreated aqueous fluids as complex as urine. Automated cryogenic concentrators permit analysis at part-per-million concentrations in environmental samples. Capillary gas chromatography interfaced to IRMS via on-line microchemistry facilitates compound-specific isotope analysis (CSIA) for purified organic analytes of 1 nmol of C, N, or O. GC-based CSIA for hydrogen and liquid chromatography-based interfaces to IRMS have both been demonstrated, and continuing progress promises to bring these advances to routine use. Automated position-specific isotope analysis (PSIA) using noncatalytic pyrolysis has been shown to produce fragments without appreciable carbon scrambling or major isotopic fractionation, and shows great promise for intramolecular isotope ratio analysis. Finally, IRMS notation and useful elementary isotopic relationships derived from the fundamental mass balance equation are presented.

    更新日期:2019-11-01
  • Mass spectrometry as a readout of protein structure and function.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1997-07-01
    R L Winston,M C Fitzgerald

    Proteins have evolved to carry out very specific functions within the cell by interacting with a diverse set of biomolecules. Understanding how a protein's higher order structure relates to its function is important for defining the molecular basis of these interactions. In recent years, mass spectrometry has become an important tool for dissecting protein structure and function. Using electrospray ionization (ESI)- and matrix-assisted laser desorption/ionization (MALDI)-based approaches, it has been possible to monitor protein folding, characterize noncovalent protein complexes, and assess the contribution of individual amino acid residues to a protein's function. Here, it is our goal to summarize these approaches and highlight recent, biologically relevant applications where mass spectrometry has provided unique insight into the mysteries of protein structure and function.

    更新日期:2019-11-01
  • Chiral recognition detected by fast atom bombardment mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1997-03-01
    M Sawada

    Detection of chiral recognition in various intermolecular interaction systems using mass spectrometry has become important for the modern fields of analytical chemistry, organic chemistry, and biochemistry due to the characteristic nature of the rapid method and the trace amount needed. This review presents the various methods for detecting and evaluating chiral recognition used primarily in fast atom bombardment mass spectrometry. Emphasis is put on fundamentals and applications of these methods for variously existing enantioselective intermolecular interaction systems.

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  • Ion-molecule reactions as probes of gas-phase structures of peptides and proteins.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1997-03-01
    M K Green,C B Lebrilla

    A review with over 100 references describes the recent applications of ion-molecule reactions to the study of gas-phase protonated peptides and proteins. The topic is focused specifically on the proton transfer and hydrogen-deuterium exchange reactions of amino acids, peptides, and proteins. A brief background is given of the various methods used for assigning proton affinities and gas-phase basicities. The methods used for measuring the kinetics of deuterium incorporation of charged ion in the presence of a background pressure of deuterating reagents are also described. Ion-molecule reactions are used to determine, among other things, the gas-phase basicities and proton affinities of amino acids, peptides, and proteins, the sites of protonation, intra- and intermolecular interactions, and conformational differences and changes in gas-phase ionic species. Singly charged and multiply charged ions are both covered.

    更新日期:2019-11-01
  • Studying noncovalent protein complexes by electrospray ionization mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 1997-01-01
    J A Loo

    Electrospray ionization mass spectrometry has been used to study protein interactions driven by noncovalent forces. The gentleness of the electrospray ionization process allows intact protein complexes to be directly detected by mass spectrometry. Evidence from the growing body of literature suggests that the ESI-MS observations for these weakly bound systems reflect, to some extent, the nature of the interaction found in the condensed phase. Stoichiometry of the complex can be easily obtained from the resulting mass spectrum because the molecular weight of the complex is directly measured. For the study of protein interactions, ESI-MS is complementary to other biophysical methods, such as NMR and analytical ultracentrifugation. However, mass spectrometry offers advantages in speed and sensitivity. The experimental variables that play a role in the outcome of ESI-MS studies of noncovalently bound complexes are reviewed. Several applications of ESI-MS are discussed, including protein interactions with metal ions and nucleic acids and subunit protein structures (quaternary structure).

    更新日期:2019-11-01
  • Selected reviews on mass spectrometric topics.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2001-02-27
    H. Budzikiewicz

    更新日期:2019-11-01
  • Perspectives for mass spectrometry and functional proteomics.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2001-02-27
    J Godovac-Zimmermann,L R Brown

    更新日期:2019-11-01
  • Applications and mechanisms of charge-remote fragmentation.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2001-02-24
    C Cheng,M L Gross

    Studies on the applications, energetics, and mechanisms of charge-remote fragmentations are reviewed, with emphasis given to those articles published after 1992. Independent of the charge status, charge-remote fragmentations are analogous to gas-phase thermolysis. Under collisional activation and with a fixed charge, ions containing long-chain or poly-ring structures undergo charge-remote fragmentations, generating productions that are structurally informative. Interpretation of the production spectra enables one to elucidate molecular structures. Although charge-remote fragmentations have been successfully used in the structural determination of fatty acids, phospholipids, glycolipids, triacylglycerols, steroids, peptides, ceramides, and other systems, the energetics and mechanisms of these reactions are still debated because none of the existing mechanisms can explain all the experimental data.

    更新日期:2019-11-01
  • New separation tools for comprehensive studies of protein expression by mass spectrometry.
    Mass Spectrom. Rev. (IF 9.068) Pub Date : 2001-02-24
    C L Nilsson,P Davidsson

    Mass spectrometry has emerged as a core technique for protein identification and characterization because of its high sensitivity, accuracy, and speed of analysis. The most widespread strategy for studying global protein expression in biological systems employs analytical two-dimensional polyacrylamide gel electrophoresis (2D PAGE) followed by enzymatic degradation of isolated protein spots, peptide mapping, and bioinformatics searches. Using this method, thousands of proteins can be resolved in a gel and their expression quantified. However, certain types of proteins possessing important cellular functions are not easily analyzed using this strategy. These proteins include membrane, low copy number, highly basic, and very large (> 150 kDa) and small (< 10 kDa) proteins. To meet the growing need to simultaneously monitor all types of proteins in a biological system, new separation strategies have emerged that are amenable to hyphenation to mass spectrometric techniques. This article will review these new techniques and examine their usefulness in studies of protein expression.

    更新日期:2019-11-01
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