Application of enriched stable isotopes as tracers in biological systems: a critical review

The application of enriched stable isotopes of minerals and trace elements as tracers in biological systems is a rapidly growing research field that benefits from the many new developments in inorganic mass spectrometric instrumentation, primarily within inductively coupled plasma mass spectrometry (ICP-MS) instrumentation, such as reaction/collision cell ICP-MS and multicollector ICP-MS with improved isotope ratio measurement and interference removal capabilities. Adaptation and refinement of radioisotope tracer experiment methodologies for enriched stable isotope experiments, and the development of new methodologies coupled with more advanced compartmental and mathematical models for the distribution of elements in living organisms has enabled a broader use of enriched stable isotope experiments in the biological sciences. This review discusses the current and future uses of enriched stable isotope experiments in biological systems.     

Polymer surface analysis: The leadership and contributions of David Briggs

David Briggs was a surface analysis pioneer. Starting in 1970 and continuing throughout his career, Dave used his expertise, vision, and ability to quickly master new surface analysis methods and solve important industrial problems. It certainly helped that he was an outstanding fundraiser in both industrial and academic settings, which ensured he always had an impressive array of the latest, most advanced surface analysis instrumentation at his disposal. He insisted on doing surface analysis correctly, and through his publications, databases, and books, he provided the community with the needed guidelines and methods to do so. In the 1970s, Dave's research was largely focused on X-ray photoelectron spectroscopy (XPS, also known as electron spectroscopy for chemical analysis [ESCA]) characterization of polymers and catalysts. He added secondary ion mass spectrometry (SIMS) to his instrumentation arsenal in the 1980s and provided many of the key, pioneering publications that described how to use this method to characterize polymer surfaces. He also did some of the first surface analysis imaging experiments in the 1980s. In the 1990s, he continued his XPS and SIMS research on polymers and advanced the surface analysis community's ability to properly interpret surface analysis data through databases and advanced data processing methods. Dave continued to publish polymer and catalysis surface analysis papers in the 2000s, but also expanded his surface analysis studies to several other topics.     

Capabilities of superpure actinide and stable isotope product in Russian Federal Nuclear Center

The paper describes the production of highly enriched isotopes of uranium, plutonium and curium by means of electromagnetic separation for scientific and applied research in physics, chemistry, geology and other field. The equipment and radiochemical methods used allows to provide the isotopic pure samples in quantities sufficient to set up nuclear physics experiments, to produce reference materials and standard sources for calibration of radiometrical and mass spectrometrical equipment and for use in radionuclear metrology. Methods of fabrication of special sources or targets and layers of highly enriched isotopes on various substrated are presented. The brief information on developing stable isotope production program is also presented.     

The use of ICPMS for stable isotope tracer studies in humans: a review

The use of stable isotope tracers in human studies is a rapidly growing research field that benefits from the many new developments in inorganic mass spectrometric instrumentation and from the better availability of mass spectrometric techniques to nutritional scientists during the last three decades. Traditionally, thermal ionization mass spectrometry (TIMS) has been the preferred technique for these studies, but the development of new inductively coupled plasma mass spectrometric (ICPMS) techniques with better isotope-ratio measurement and interference-removal capabilities (e.g. single and multi-detector ICPMS and reaction/collision cell ICPMS) has enabled broader use of ICPMS for determination of stable isotope tracers in nutritional research. This review discusses the current and future use of ICPMS in stable isotope tracer studies in humans.     

Airborne mass spectrometers: four decades of atmospheric and space research at the Air Force research laboratory.

Mass spectrometry is a versatile research tool that has proved to be extremely useful for exploring the fundamental nature of the earth's atmosphere and ionosphere and in helping to solve operational problems facing the Air Force and the Department of Defense. In the past 40 years, our research group at the Air Force Research Laboratory has flown quadrupole mass spectrometers of many designs on nearly 100 sounding rockets, nine satellites, three Space Shuttles and many missions of high-altitude research aircraft and balloons. We have also used our instruments in ground-based investigations of rocket and jet engine exhaust, combustion chemistry and microwave breakdown chemistry. This paper is a review of the instrumentation and techniques needed for space research, a summary of the results from many of the experiments, and an introduction to the broad field of atmospheric and space mass spectrometry in general.     

Developing front‐end devices for improved sample preparation in MS‐based proteome analysis

Chemical analysis has long relied on instrumentation, from the simplest (eg, burets) to the more sophisticated (eg, mass spectrometers) to facilitate precision measurements. Regardless of their complexity, the development of a new instrumental device can be a valued approach to address problems in science. In this perspective, we outline the process of novel device design, from early phase conception to the manufacturing and testing of the tool or gadget. Focus is placed on the development of improved front‐end devices to facilitate protein sample manipulations ahead of mass spectrometry, which therefore augment the proteomics workflow. Highlighted are some of the many training secrets, choices, and challenges that are inherent to the often iterative process of device design. In hopes of inspiring others to pursue instrument design to address relevant research questions, we present a summary list of points to consider prior to innovating their own devices.     

现代固态有机化学之父——Gerhard M.J.Schmidt

本文主要介绍了GerhardM.J.Schmidt教授的生平、代表性的科研工作及其意义、影响和应用,从中展现出他的优秀品质、治学精神、杰出成就以及影响力。Schmidt教授少年早慧,求学艰辛,天赋独特,痴迷科学,为科学事业奋斗终身,在多个领域都有着卓越的成就,其中以固态有机化学领域最具代表性。他在科研的同时还担任诸多行政职务,为魏茨曼研究所、以色列乃至全世界的科学发展做了许多贡献。     

Compound-specific stable isotope analysis of organic contaminants in natural environments: a critical review of the state of the art,prospects, and future challenges

Compound-specific stable isotope analysis (CSIA) using gas chromatography-isotope ratio mass spectrometry (GC/IRMS) has developed into a mature analytical method in many application areas over the last decade. This is in particular true for carbon isotope analysis, whereas measurements of the other elements amenable to CSIA (hydrogen, nitrogen, oxygen) are much less routine. In environmental sciences, successful applications to date include (i) the allocation of contaminant sources on a local, regional, and global scale, (ii) the identification and quantification of (bio)transformation reactions on scales ranging from batch experiments to contaminated field sites, and (iii) the characterization of elementary reaction mechanisms that govern product formation. These three application areas are discussed in detail. The investigated spectrum of compounds comprises mainly n-alkanes, monoaromatics such as benzene and toluene, methyl tert-butyl ether (MTBE), polycyclic aromatic hydrocarbons (PAHs), and chlorinated hydrocarbons such as tetrachloromethane, trichloroethylene, and polychlorinated biphenyls (PCBs). Future research directions are primarily set by the state of the art in analytical instrumentation and method development. Approaches to utilize HPLC separation in CSIA, the enhancement of sensitivity of CSIA to allow field investigations in the µg L^–1 range, and the development of methods for CSIA of other elements are reviewed. Furthermore, an alternative scheme to evaluate isotope data is outlined that would enable estimates of position-specific kinetic isotope effects and, thus, allow one to extract mechanistic chemical and biochemical information.Abbreviations BTEX benzene, toluene, ethylbenzene, xylenes - MTBE methyl tert-butyl ether - PAHs polycyclic aromatic hydrocarbons - VOCs volatile compounds - PCBs polychlorinated biphenyls - CSIA compound-specific (stable) isotope (ratio) analysis - GC-IRMS, GC/IRMS or GCIRMS gas chromatography-isotope ratio mass spectrometry - GC-C-IRMS, GC/C/IRMS or GCC-IRMS gas chromatography-combustion-isotope ratio mass spectrometry - irmGC/MS isotope ratio monitoring gas chromatograph-mass spectrometry - GC/P/IRMS gas chromatography-pyrolysis-isotope ratio mass spectrometry (used for D/H) - KIE kinetic isotope effect - PSIA position-specific isotope analysis (for intramolecular isotope distribution) - SNIF-NMR site-specific natural isotopic fractionation by nuclear magnetic resonance spectroscopy     

Mass spectrometry of long-lived radionuclides

The capability of determining element concentrations at the trace and ultratrace level and isotope ratios is a main feature of inorganic mass spectrometry. The precise and accurate determination of isotope ratios of long-lived natural and artificial radionuclides is required, e.g. for their environmental monitoring and health control, for studying radionuclide migration, for age dating, for determining isotope ratios of radiogenic elements in the nuclear industry, for quality assurance and determination of the burn-up of fuel material in a nuclear power plant, for reprocessing plants, nuclear material accounting and radioactive waste control. Inorganic mass spectrometry, especially inductively coupled plasma mass spectrometry (ICP-MS) as the most important inorganic mass spectrometric technique today, possesses excellent sensitivity, precision and good accuracy for isotope ratio measurements and practically no restriction with respect to the ionization potential of the element investigated—therefore, thermal ionization mass spectrometry (TIMS), which has been used as the dominant analytical technique for precise isotope ratio measurements of long-lived radionuclides for many decades, is being replaced increasingly by ICP-MS. In the last few years instrumental progress in improving figures of merit for the determination of isotope ratio measurements of long-lived radionuclides in ICP-MS has been achieved by the application of a multiple ion collector device (MC-ICP-MS) and the introduction of the collision cell interface in order to dissociate disturbing argon-based molecular ions, to reduce the kinetic energy of ions and neutralize the disturbing noble gas ions (e.g. of ¹²⁹Xe⁺ for the determination of ¹²⁹I). The review describes the state of the art and the progress of different inorganic mass spectrometric techniques such as ICP-MS, laser ablation ICP-MS vs. TIMS, glow discharge mass spectrometry, secondary ion mass spectrometry, resonance ionization mass spectrometry and accelerator mass spectrometry for the determination of long-lived radionuclides in quite different materials.     

快速蒸发电离质谱技术及其应用研究进展

近年来,原位电离质谱技术成为质谱分析领域的研究前沿和热点.快速蒸发电离质谱技术源于外科手术中的手术烟雾现象,自2009年报道以来,作为一种新型原位电离质谱技术已被广泛应用于医学、微生物鉴定、食品真伪鉴别、代谢物研究、药用植物成分鉴定等领域.该技术通过电离切割组织或其他生物样品产生的含丰富特定区域生物特征的气溶胶,对其进...     

Prototyping an ionization source for non-engineers

Novel mass spectrometry (MS) based analytical platforms have enabled scientists to detect and quantify molecules within biological and environmental samples more accurately. Novel MS instrumentation starts as a prototype and, after years of development, can become a commercial product to be used by the larger MS community. Without the initial prototype, many MS-based instruments today would not be produced. Additionally, biotechnology companies are the main drivers for research, development, and production of novel instruments, but the tools for prototyping instrumentation have never been more accessible. Here, we present a tutorial on prototyping instrumentation through the case study of developing the Next Generation IR-MALDESI source to show that an engineering degree is not required to design and construct a prototype instrument with modern hardware and software. We discuss the prototyping process, the necessary skills required for efficient prototyping, and information about common hardware and software used within initial prototypes.     

Paradigms in isotope dilution mass spectrometry for elemental speciation analysis

Isotope dilution mass spectrometry currently stands out as the method providing results with unchallenged precision and accuracy in elemental speciation. However, recent history of isotope dilution mass spectrometry has shown that the extent to which this primary ratio measurement method can deliver accurate results is still subject of active research. In this review, we will summarize the fundamental prerequisites behind isotope dilution mass spectrometry and discuss their practical limits of validity and effects on the accuracy of the obtained results. This review is not to be viewed as a critique of isotope dilution; rather its purpose is to highlight the lesser studied aspects that will ensure and elevate current supremacy of the results obtained from this method.     

The graphite furnace and its role in atomic spectroscopy

The diversity of applications of the graphite furnace is extraordinary, encompassing the fields of physics, thermochemistry, spectroscopy and analytical chemistry. In this respect, the graphite furnace has been used on a continuous basis as a research tool for nearly a century. Following its introduction as an atomization source for atomic absorption spectrometry by L'vov in 1959, its role in atomic spectrometry expanded considerably to encompass analytical applications in emision, fluorescence, absorption and mass spectrometry. In addition to its conspicuous use as an atomization source in these areas, it is frequently employed as a vaporizer when used in the format of combined and tandem sources with other instrumentation. The unique physico-chemical micro-environment which can be attained within the graphite furnace has also been used to advantage in a number of investigations, including the determination of gas- and solid-phase diffusion coefficients of high-temperature metal vapours, the heats of sublimation of refractory metals, fundamental optical constants and the measurement of the heats of desorption of adatoms from high-temperature surfaces. The range of such applications remains to be more fully explored. The attractive features of this source, viz., the high atomization/vaporization efficiency, comparatively long atomic vapour residence times, controllable chemical and thermal environment and its ability to handle high dissolved solids content samples (相似文献   

An appreciation of the scientific researches of Dr Peter H. Dawson

Upon the death of Peter H. Dawson in 2015, mass spectrometry lost a major figure. Within the area of radiofrequency quadrupole electric fields applied to mass spectrometry, Dawson stands alongside its pioneers Wolfgang Paul, Nobelist and inventor of the technology, and Wilson Brubaker, who identified and overcame the deleterious effects of fringing electric fields on quadrupole mass filter performance. Seventy‐one of Dawson's 97 scientific publications are concerned with quadrupole mass analysers, ion traps and monopole mass spectrometers. Of especial note are his book and review articles in which he disseminated information on the theoretical fundamentals and practicalities of these systems to a wider audience, thereby having a major impact on the development of this important field of endeavour. The scientific researches of Dr Dawson, and his advice and counsel, influenced to a major degree, and to the better, the research careers, teachings and the lives of the authors of this piece. Their combined researches on quadrupole devices led to the commercialization of the ion trap as a mass spectrometer by which mass spectral information became available at greatly reduced cost. Thus, the advent of commercial ion trapping instruments permitted a greater use of mass spectrometry in both technically advanced countries and those less well advanced. The greatest impact in health services was mass spectrometric analysis of environmental problems, well and stream water, food free of pesticides, etc., and forensic sciences. Our combined indebtedness to Dr Dawson is manifested by this appreciation of his scientific work, the highlighting of his main contributions, and creation of a substantive reference source to his work that can be used by other scientists. A comprehensive list of Dr Dawson's publications, including abstracts or summaries, has been arranged in chronological order of date of submission.     

The scientific legacy of Howard Vincent Malmstadt

Howard Malmstadt was a true giant of Analytical Chemistry and clearly one of the most influential analytical chemists of the last 50 years. Howard, through his own work and that of his students (first generation) and their students (second generation) and their students' students (third generation) changed the course of Analytical Chemistry. His research interests were broad and ranged from analytical solution chemistry (titrimetry and reaction rates) and electrochemistry to atomic and molecular spectroscopy, chemical instrumentation, clinical chemistry and automation. Howard was also one of the most innovative and influential educators of our time. He changed forever the analytical curriculum through his many books on Electronics for Scientists, most written in conjunction with Chris Enke and Stan Crouch. Their texts and short courses went from pioneering the application of tube-based analog electronics (servo systems and operational amplifiers) in scientific measurements to the impact that integrated circuits and digital electronics would have on laboratory measurements. He strongly believed in the importance of “hands-on” in education. To this end, he expended considerable personal effort and time to see not only the development and commercialization of an effective laboratory infrastructure to support education in analog and digital electronics, but also oversaw the development of modular instrumentation for spectroscopy. Over the years he received many awards from the Analytical Chemistry community for his outstanding efforts and contributions to teaching and research. Many of Howard's students went on into academia. They and their students now represent the ongoing legacy for analytical chemistry that evolved from Howard's laboratory at Illinois. A remarkable diversity of research programs are underway in their laboratories. Topics range from atomic, laser, mass, and Raman spectroscopy to detection technology, analytical education, micro-fabricated instrumentation, and intercellular analytical measurements.     

Progress of laser ionization mass spectrometry for elemental analysis — A review of the past decade

Mass spectrometry using a laser ionization source has played a significant role in elemental analysis. Three types of techniques are widely used: high irradiance laser ionization mass spectrometry is capable of rapid determination of elements in solids; single particle mass spectrometry is a powerful tool for single particle characterization; and resonance ionization mass spectrometry is applied for isotope ratio measurements with high sensitivity and selectivity. In this review, the main features of the laser ablation process and plasma characterization by mass spectrometry are summarized. Applications of these three techniques for elemental analysis are discussed.     

An introduction to hybrid ion trap/time‐of‐flight mass spectrometry coupled with liquid chromatography applied to drug metabolism studies

Metabolism studies play an important role at various stages of drug discovery and development. Liquid chromatography combined with mass spectrometry (LC/MS) has become a most powerful and widely used analytical tool for identifying drug metabolites. The suitability of different types of mass spectrometers for metabolite profiling differs widely, and therefore, the data quality and reliability of the results also depend on which instrumentation is used. As one of the latest LC/MS instrumentation designs, hybrid ion trap/time‐of‐flight MS coupled with LC (LC‐IT‐TOF‐MS) has successfully integrated ease of operation, compatibility with LC flow rates and data‐dependent MSⁿ with high mass accuracy and mass resolving power. The MSⁿ and accurate mass capabilities are routinely utilized to rapidly confirm the identification of expected metabolites or to elucidate the structures of uncommon or unexpected metabolites. These features make the LC‐IT‐TOF‐MS a very powerful analytical tool for metabolite identification. This paper begins with a brief introduction to some basic principles and main properties of a hybrid IT‐TOF instrument. Then, a general workflow for metabolite profiling using LC‐IT‐TOF‐MS, starting from sample collection and preparation to final identification of the metabolite structures, is discussed in detail. The data extraction and mining techniques to find and confirm metabolites are discussed and illustrated with some examples. This paper is directed to readers with no prior experience with LC‐IT‐TOF‐MS and will provide a broad understanding of the development and utility of this instrument for drug metabolism studies. Copyright © 2012 John Wiley & Sons, Ltd.     

Radioanalytical chemistry for nuclear forensics in China: Progress and future perspective

A relatively new branch of science - nuclear forensics, aiming at providing the nature, origin, history and possible trafficking route of seized nuclear materials/devices, has been established and rapidly developed over decades to screen illicit nuclear activities. This highly interdisciplinary science is built upon a foundation of analytical chemistry, radiochemistry, nuclear physics, material sciences, geology, and other scientific disciplines, within which radiochemical methodologies and radioanalytical techniques play a key role. The present review provides a brief overview about the crucial aspects of nuclear forensics, including basic content, procedure, concerned elements, common separation, analytical method, and so on. The state of the art and recent progresses of nuclear forensics by research communities in China are reviewed, while selected examples and practical applications are emphasized. The challenges associated with this new area and on-going developments are highlighted and discussed.     

Capillary electrophoresis inductively coupled plasma mass spectrometry

Chemical speciation (extraction of elemental information and identification of molecular environment for an analyte in a complex sample) has been a long sought after goal for analytical chemists. Recently, because of successful developments in more sensitive element-specific detectors and gentle separation schemes, which preserve the true chemical information in a real sample, routine speciation experiments are becoming a common occurrence in the scientific literature. For many reasons, the combination of capillary electrophoresis (for separation of different chemical species) with inductively coupled plasma mass spectrometry (for element and isotope specific detection) has emerged as the method of choice for these analyses. In this article the basic principles of capillary electrophoresis inductively coupled plasma mass spectrometry are discussed. Design consideration for instrument interface, anticipated difficulties with speciation experiments and applications for specific matrices and analytes are also presented in this article.     

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