著者
Britt S.R. Claes Emi Takeo Eiichiro Fukusaki Shuichi Shimma Ron M.A. Heeren
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
pp.A0078, (Released:2019-11-06)
参考文献数
119
被引用文献数
4

Mass spectrometry imaging is an imaging technology that allows the localization and identification of molecules on (biological) sample surfaces. Obtaining the localization of a compound in tissue is of great value in biological research. Yet, the identification of compounds remains a challenge. Mass spectrometry alone, even with high-mass resolution, cannot always distinguish between the subtle structural differences of isomeric compounds. This review discusses recent advances in mass spectrometry imaging of lipids, steroid hormones, amino acids and proteins that allow imaging with isomeric resolution. These improvements in detailed identification can give new insights into the local biological activity of isomers.
著者
Lee Chuin Chen Kentaro Yoshimura Satoshi Ninomiya Sen Takeda Kenzo Hiraoka
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.6, no.3, pp.S0070-S0070, 2017-08-25 (Released:2017-08-23)
参考文献数
42
被引用文献数
2

In this paper, we briefly review the remote mass spectrometric techniques that are viable to perform “endoscopic mass spectrometry,” i.e., in-situ and in-vivo MS analysis inside the cavity of human or animal body. We also report our experience with a moving string sampling probe for the remote sample collection and the transportation of adhered sample to an ion source near the mass spectrometer. With a miniaturization of the probe, the method described here has the potential to be fit directly into a medical endoscope.
著者
Britt S. R. Claes Emi Takeo Eiichiro Fukusaki Shuichi Shimma Ron M. A. Heeren
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.8, no.1, pp.A0078, 2019-12-27 (Released:2019-12-28)
参考文献数
119
被引用文献数
4

Mass spectrometry imaging is an imaging technology that allows the localization and identification of molecules on (biological) sample surfaces. Obtaining the localization of a compound in tissue is of great value in biological research. Yet, the identification of compounds remains a challenge. Mass spectrometry alone, even with high-mass resolution, cannot always distinguish between the subtle structural differences of isomeric compounds. This review discusses recent advances in mass spectrometry imaging of lipids, steroid hormones, amino acids and proteins that allow imaging with isomeric resolution. These improvements in detailed identification can give new insights into the local biological activity of isomers.
著者
Mark Beattie Oliver A. H. Jones
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.12, no.1, pp.A0118, 2023-04-06 (Released:2023-04-06)
参考文献数
40

Mass spectrometry is a well-established analytical technique for studying the masses of atoms, molecules, or fragments of molecules. One of the key metrics of mass spectrometers is the limit of detection e.g., the minimum amount of signal from an analyte that can be reliably distinguished from noise. Detection limits have improved greatly over the last 30–40 years to the point that nanogram per litre and even picogram per litre detections are commonly reported. There is however, a difference between detection limits obtained with a single, pure compound in a pure solvent and those obtained from real life samples/matrixes. Determining a practical detection limit for mass spectrometry is difficult because it depends on multiple factors, such as the compound under test, the matrix, data processing methods and spectrometer type. Here we show the improvements in reported limits of detection on mass spectrometers over time using industry and literature data. The limit of detection for glycine and dichlorodiphenyltrichloroethane were taken from multiple published articles spanning a period of 45 years. The limits of detection were plotted against the article’s year of publication to assess whether the trend in improvement in sensitivity resembles Moore’s Law of computing (essentially doubling every two years). The results show that advancements in detection limits in mass spectrometry are close to, but not quite at a rate equivalent to Moore’s Law and the improvements in detection limits reported from industry seem to be greater than those reported in the academic literature.
著者
Robert B. Cody
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.2, no.Special_Issue, pp.S0007, 2013-04-15 (Released:2013-05-03)
参考文献数
33
被引用文献数
4 9

The introduction of DART and DESI sources approximately seven years ago led to the development of a new series of atmospheric pressure ion sources referred to as “ambient ionization” sources. These fall into two major categories: spray techniques like DESI or plasma techniques like DART. The selectivity of “direct ionization,” meaning analysis without chromatography and with little or no sample preparation, depends on the mass spectrometer selectivity. Although high resolution and tandem mass spectrometry are valuable tools, rapid and simple sample preparation methods can improve the utility of ambient ionization methods. The concept of ambient ionization has led to the realization that there are many more ways to form ions than might be expected. An interesting example is the use of a flint-and-steel spark source to generate ions from compounds such as phenolphthalein and Gramicidin S.
著者
Yuko Nakashima Mitsutoshi Setou
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.7, no.1, pp.A0070, 2018-09-11 (Released:2018-09-11)
参考文献数
37
被引用文献数
16

Oligonucleotide-based therapeutics such as antisense oligonucleotides, small interfering RNAs (siRNAs), decoy and aptamer have been extensively developed. To investigate the pharmacokinetics of oligonucleotide therapeutics, it is common to label a radioisotope in a nucleic acid and visualize it. However, if the labeled terminal nucleotide is decomposed by a nuclease in vivo, only the labeled nucleotide is detected, and it is impossible to observe the nucleic acid exhibiting the drug effect. The distribution of biomolecules, such as phospholipids, proteins, and glycolipids, can be obtained and visualized without labeling using matrix-assisted laser desorption/ionization imaging mass spectrometry (MALDI-IMS). MALDI-IMS is also used in pharmacokinetic analysis to visualize a parent drug and its metabolites simultaneously. In this study, we reported a methodology for oligonucleotides analysis by MALDI-IMS. When phosphorothioate antisense oligonucleotide was administered into the eyeball of rats, it reached the retina after 30 min without undergoing decomposition by nucleases.
著者
Yukina Tatsuta Yukie Tanaka Akari Ikeda Shigeru Matsukawa Hajime Katano Shu Taira
出版者
日本質量分析学会
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.6, no.3, pp.S0069-S0069, 2017-09-08 (Released:2017-09-15)
参考文献数
7
被引用文献数
8

We compared two ionization methods, matrix assisted laser desorption/ionization (MALDI) and nanoparticle assisted laser desorption/ionization (Nano-PALDI) mass spectrometry (MS), for the analysis of amino acids derivatized with Py-Tag™ that consists pyrylium-based compound. Py-Tag is a useful stable derivatization reagent due to wide mass differences (using 13C as the sole stable labelling isotope). For Py-Tag labelled lysine, sensitive signals that showed less noise with a ten times higher sensitivity, showed a wider mass difference by Nano-PALDI MS compared to MALDI MS.
著者
Anil Kumar Meher Yu-Chie Chen
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.6, no.2, pp.S0057-S0057, 2017-03-18 (Released:2017-03-24)
参考文献数
147
被引用文献数
4 15

Generation of analyte ions in gas phase is a primary requirement for mass spectrometric analysis. One of the ionization techniques that can be used to generate gas phase ions is electrospray ionization (ESI). ESI is a soft ionization method that can be used to analyze analytes ranging from small organics to large biomolecules. Numerous ionization techniques derived from ESI have been reported in the past two decades. These ion sources are aimed to achieve simplicity and ease of operation. Many of these ionization methods allow the flexibility for elimination or minimization of sample preparation steps prior to mass spectrometric analysis. Such ion sources have opened up new possibilities for taking scientific challenges, which might be limited by the conventional ESI technique. Thus, the number of ESI variants continues to increase. This review provides an overview of ionization techniques based on the use of electrospray reported in recent years. Also, a brief discussion on the instrumentation, underlying processes, and selected applications is also presented.
著者
Sy-Chyi Cheng Shih-His Chen Jentaie Shiea
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.6, no.2, pp.S0065-S0065, 2017-03-18 (Released:2017-03-24)
参考文献数
43
被引用文献数
8

Flame-induced atmospheric pressure chemical ionization (FAPCI) is a solvent and high voltage-free APCI technique. It uses a flame to produce charged species that reacts with analytes for ionization, and generates intact molecular ions from organic compounds with minimal fragmentation. In this study, desorption FAPCI/MS was developed to rapidly characterize thermally stable organic compounds in liquid, cream, and solid states. Liquid samples were introduced into the ion source through a heated nebulizer, and the analytes formed in the heated nebulizer reacted with charged species in the source. For cream and solid sample analysis, the samples were positioned near the flame of the FAPCI source for thermal desorption and ionization. This approach provided a useful method to directly characterize samples with minimal pretreatment. Standards and real-world samples, such as drug tablets, ointment, and toy were analyzed to demonstrate the capability of desorption FAPCI/MS for rapid organic compound analysis.
著者
Li-Hua Li Hua-Yi Hsieh Cheng-Chih Hsu
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.6, no.2, pp.S0060-S0060, 2017-02-22 (Released:2017-02-24)
参考文献数
100
被引用文献数
31

Ambient ionization allows mass spectrometry analysis directly on the sample surface under atmospheric pressure with almost zero sample pretreatment. Since the development of desorption electrospray ionization (DESI) in 2004, many other ambient ionization techniques were developed. Due to their simplicity and low operation cost, rapid and on-site clinical mass spectrometry analysis becomes real. In this review, we will highlight some of the most widely used ambient ionization mass spectrometry approaches and their applications in clinical study.
著者
Peter S. Haglund Karin Löfstrand Kevin Siek Lillemor Asplund
出版者
日本質量分析学会
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.2, no.Special_Issue, pp.S0018-S0018, 2013-04-15 (Released:2013-05-03)
参考文献数
23
被引用文献数
4 13

Comprehensive two-dimensional gas chromatography/time-of-flight mass spectrometry (GC×GC TOFMS) and gas chromatography/high-resolution time-of-flight mass spectrometry (GC-HRT) were used to detect and identify halogenated natural products (HNPs) in tissue homogenate, in this case brominated analytes present in a marine snail. Two classes of brominated anthropogenic compounds, polybrominated diphenyl ethers (PBDEs) and brominated dibenzofurans, were analyzed for comparison. Following conventional preparation, the sample was analyzed using GC×GC-TOF-MS. Isotope ratio scripts were used to compile a list of putatively brominated analytes from amongst the thousands of features resolved in the two-dimensional chromatogram. The structured nature of the chromatogram was exploited to propose identifications for several classes of brominated compounds, and include additional candidates that fell marginally outside the script tolerances. The sample was subsequently analyzed by GC-HRT. The high-resolution mass spectral data confirmed many formula assignments, facilitated confident assignment of an alternate formula when an original proposal did not hold, and enabled unknown identification. Identified HNPs include hydroxylated and methoxylated PBDE analogs, polybrominated dibenzo-p-dioxins (PBDDs) and hydroxyl-PBDDs, permitting the environmental occurrence and fate of such compounds to be studied.
著者
Fumio Matsuda Shuka Komori Yuki Yamada Daiki Hara Nobuyuki Okahashi
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
pp.A0106, (Released:2022-11-05)
参考文献数
44
被引用文献数
1

In metabolomics studies using high-resolution mass spectrometry (MS), a set of product ion spectra is comprehensively acquired from observed ions using the data-dependent acquisition (DDA) mode of various tandem MS. However, especially for low-intensity signals, it is sometimes difficult to distinguish artifact signals from true fragment ions derived from a precursor ion. Inadequate precision in the measured m/z value is also one of the bottlenecks to narrowing down the candidate compositional formula. In this study, we report that averaging multiple product ion spectra can improve m/z precision as well as the reliability of fragment ions that are observed in such spectra. A graph-based method was applied to cluster a set of similar spectra from multiple DDA data files resulting in creating an averaged product-ion spectrum. The error levels for the m/z values declined following the central limit theorem, which allowed us to reduce the number of candidate compositional formulas. The improved reliability and precision of the averaged spectra will contribute to a more efficient annotation of product ion spectral data.
著者
Shuichi Shimma
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.11, no.1, pp.A0102, 2022-02-25 (Released:2022-02-25)
参考文献数
32
被引用文献数
3

Mass spectrometry imaging (MSI) is a technique for obtaining information on the distribution of various molecules by performing mass spectrometry directly on the sample surface. The applications range from small molecules such as lipids to large molecules such as proteins. It is also possible to detect pharmaceuticals and elemental isotopes in interstellar matter. This review will introduce various applications of MSI with examples.
著者
Kosuke Ogata Chih-Hsiang Chang Yasushi Ishihama
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
pp.A0093, (Released:2020-12-11)
参考文献数
47
被引用文献数
13

The insertion of ion mobility spectrometry (IMS) between LC and MS can improve peptide identification in both proteomics and phosphoproteomics by providing structural information that is complementary to LC and MS, because IMS separates ions on the basis of differences in their shapes and charge states. However, it is necessary to know how phosphate groups affect the peptide collision cross sections (CCS) in order to accurately predict phosphopeptide CCS values and to maximize the usefulness of IMS. In this work, we systematically characterized the CCS values of 4,433 pairs of mono-phosphopeptide and corresponding unphosphorylated peptide ions using trapped ion mobility spectrometry (TIMS). Nearly one-third of the mono-phosphopeptide ions evaluated here showed smaller CCS values than their unphosphorylated counterparts, even though phosphorylation results in a mass increase of 80 Da. Significant changes of CCS upon phosphorylation occurred mainly in structurally extended peptides with large numbers of basic groups, possibly reflecting intramolecular interactions between phosphate and basic groups.
著者
Takafumi Hirata Shuji Yamashita Mirai Ishida Toshihiro Suzuki
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.9, no.1, pp.A0085, 2020-06-10 (Released:2020-06-12)
参考文献数
45
被引用文献数
12

We measured the Re/Os (185Re/188Os) and 187Os/188Os ratios from nanoparticles (NPs) using a multiple collector-inductively coupled plasma-mass spectrometer equipped with high-time resolution ion counters (HTR-MC-ICP-MS). Using the HTR-MC-ICP-MS system developed in this study, the simultaneous data acquisition of four isotopes was possible with a time resolution of up to 10 μs. This permits the quantitative analysis of four isotopes to be carried out from transient signals (e.g., <0.6 ms) emanating from the NPs. Iridium–Osmium NPs were produced from a naturally occurring Ir–Os alloy (ruthenosmiridium from Hokkaido, Japan; osmiridium from British Columbia, Canada; iridosmine from the Urals region of Russia) through a laser ablation technique, and the resulting nanoparticles were collected by bubbling water through a suspension. The 187Os/188Os ratios for individual NPs varied significantly, mainly due to the counting statistics of the 187Os and 188Os signals. Despite the large variation in the measured ratios, the resulting 187Os/188Os ratios for three Ir–Os bearing minerals, were 0.121±0.013 for Hokkaido, 0.110±0.012 for British Columbia, and 0.122±0.020 for the Urals, and these values were in agreement with the ratios obtained by the conventional laser ablation-MC-ICP-MS technique. The data obtained here provides a clear demonstration that the HTR-MC-ICP-MS technique can become a powerful tool for monitoring elemental and isotope ratios from NPs of multiple components.
著者
Kohta Nakatani Yoshihiro Izumi Kosuke Hata Takeshi Bamba
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.9, no.1, pp.A0080, 2020-03-17 (Released:2020-03-17)
参考文献数
26
被引用文献数
25

The rapid development of next-generation sequencing techniques has enabled single-cell genomic and transcriptomic analyses, which have revealed the importance of heterogeneity in biological systems. However, analytical methods to accurately identify and quantify comprehensive metabolites from single mammalian cells with a typical diameter of 10–20 μm are still in the process of development. The aim of this study was to develop a single-cell metabolomic analytical system based on highly sensitive nano-liquid chromatography tandem mass spectrometry (nano-LC-MS/MS) with multiple reaction monitoring. A packed nano-LC column (3-μm particle-size pentafluorophenylpropyl Discovery HSF5 of dimensions 100 μm i.d.×180 mm) was prepared using a slurry technique. The optimized nano-LC-MS/MS method showed 3–132-fold (average value, 26-fold) greater sensitivity than semimicro-LC-MS/MS, and the detection limits for several hydrophilic metabolites, including amino acids and nucleic acid related metabolites were in the sub-fmol range. By combining live single-cell sampling and nano-LC-MS/MS, we successfully detected 18 relatively abundant hydrophilic metabolites (16 amino acids and 2 nucleic acid related metabolites) from single HeLa cells (n=22). Based on single-cell metabolic profiles, the 22 HeLa cells were classified into three distinct subclasses, suggesting differences in metabolic function in cultured HeLa cell populations. Our single-cell metabolomic analytical system represents a potentially useful tool for in-depth studies focused on cell metabolism and heterogeneity.
著者
Dilshadbek Tursunbayevich Usmanov Satoshi Ninomiya Lee Chuin Chen Subhrakanti Saha Mridul Kanti Mandal Yuji Sakai Rio Takaishi Ahsan Habib Kenzo Hiraoka Kentaro Yoshimura Sen Takeda Hiroshi Wada Hiroshi Nonami
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.6, no.2, pp.S0059-S0059, 2017-02-24 (Released:2017-02-24)
参考文献数
89
被引用文献数
9

In mass spectrometry, analytes must be released in the gas phase. There are two representative methods for the gasification of the condensed samples, i.e., ablation and desorption. While ablation is based on the explosion induced by the energy accumulated in the condensed matrix, desorption is a single molecular process taking place on the surface. In this paper, desorption methods for mass spectrometry developed in our laboratory: flash heating/rapid cooling, Leidenfrost phenomenon-assisted thermal desorption (LPTD), solid/solid friction, liquid/solid friction, electrospray droplet impact (EDI) ionization/desorption, and probe electrospray ionization (PESI), will be described. All the methods are concerned with the surface and interface phenomena. The concept of how to desorb less-volatility compounds from the surface will be discussed.
著者
Yuki Yamada Satoshi Ninomiya Kenzo Hiraoka Lee Chuin Chen
出版者
The Mass Spectrometry Society of Japan
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.5, no.2, pp.S0068-S0068, 2017-04-18 (Released:2017-04-27)
参考文献数
23
被引用文献数
5

We report on combining a self-aspirated sampling probe and an ESI source using a single metal capillary which is electrically grounded and safe for use by the operator. To generate an electrospray, a negative H.V. is applied to the counter electrode of the ESI emitter to operate in positive ion mode. The sampling/ESI capillary is enclosed within another concentric capillary similar to the arrangement for a standard pneumatically assisted ESI source. The suction of the liquid sample is due to the Venturi effect created by the high-velocity gas flow near the ESI tip. In addition to serving as the mechanism for suction, the high-velocity gas flow also assists in the nebulization of charged droplets, thus producing a stable ion signal. Even though the potential of the ion source counter electrode is more negative than the mass spectrometer in the positive ion mode, the electric field effect is not significant if the ion source and the mass spectrometer are separated by a sufficient distance. Ion transmission is achieved by the viscous flow of the carrier gas. Using the present arrangement, the user can hold the ion source in a bare hand and the ion signal appears almost immediately when the sampling capillary is brought into contact with the liquid sample. The automated analysis of multiple samples can also be achieved by using motorized sample stage and an automated ion source holder.
著者
Fumio Matsuda
出版者
日本質量分析学会
雑誌
Mass Spectrometry (ISSN:2187137X)
巻号頁・発行日
vol.3, no.Special_Issue_2, pp.S0038-S0038, 2014-08-01 (Released:2014-08-16)
参考文献数
38
被引用文献数
4 14

The CASMI 2013 (Critical Assessment of Small Molecule Identification 2013, http://casmi-contest.org/) contest was held to systematically evaluate strategies used for mass spectrometry-based identification of small molecules. The results of the contest highlight that, because of the extensive efforts made towards the construction of databases and search tools, database-assisted small molecule identification can now automatically annotate some metabolite signals found in the metabolome data. In this commentary, the current state of metabolite annotation is compared with that of transcriptomics and proteomics. The comparison suggested that certain limitations in the metabolite annotation process need to be addressed, such as (i) the completeness of the database, (ii) the conversion between raw data and structure, (iii) the one-to-one correspondence between measured data and correct search results, and (iv) the false discovery rate in database search results.