摘要:In recent years,ambient ionization mass spectrometry(AIMS) has become a frontier research and hotspot in the field of mass spectrometry analysis.Since first reported in 2009 as a new AIMS technique,rapid evaporative ionization mass spectrometry(REIMS),originating from the phenomenon of surgical smoke in surgery operation,has been widely used in medical science,microorganism characterization,food authenticity identification,metabolites study,and medicinal plant ingredients analysis.By cutting and ionizing tissues or other biological samples,REIMS could be used to generate aerosols with rich biological characteristics of specific regions for in situ,online,real time,and rapid mass spectrometry analysis.The development history,ionization mechanism,working principle,and applications of REIMS in different fields are reviewed in the present work,which could provide scientific inspiration and technical guidance for relevant researchers.  
关键词:rapid evaporative ionization mass spectrometry;ambient ionization;review
摘要:In recent years,the rapid development of sample pretreatment techniques interfaced with direct analysis in real-time mass spectrometry(DART-MS) has allowed for the direct analysis on target analytes in complex biological,environmental,forensic and food environments,as well as individual small organisms and single cell samples.However,difficulties in detecting the internal analytes in solid matrices and the poor detection performance of trace analytes have become key problems restricting the further development of DART-MS.To solve these problems,several attempts have been made in different research fields to combine sample pretreatment methods with MS.The combinations of sample pretreatment techniques,such as solid-phase extraction(SPE),dispersive solid-phase extraction(DSPE),stir bar sorptive extraction(SBSE),solid-phase microextraction(SPME),mechanochemical extraction(MCE) and microwave-assisted extraction(MAE) with DART-MS are summarized in this review.The improvements that these combined methods may offer are detailed,and the future development trends are also proposed.It is hoped that this review will provide a reference or a basis for the future advancement of new sample treatment techniques in combination with DART-MS.  
关键词:ambient ionization mass spectrometry;direct analysis in real time mass spectrometry(DART-MS);sample pretreatment technique;review
摘要:Ambient ionization mass spectrometry is a novel and rapid mass spectrometric technique with the characteristics of rapid analysis,simple operation and high specificity.This technique integrated with a miniature mass spectrometer could be performed to achieve the rapid screening and accurate analysis of samples without any complex sample pretreatment,showing a great potential in the screening of chemical risk substances in trade products.This review mainly focuses on the recent research progresses of ambient mass spectrometry on the screening of chemical risk substances in trade products.The future development and potential applications of ambient ionization mass spectrometry are also discussed.  
摘要:Ambient laser based ionization mass spectrometry has characteristics such as high spatial resolution,simple sample pretreatment,easy portability and accessibility of imaging analysis,etc.Matrix assisted laser ionization source mass spectrometry has been widely used in the analysis of biomacromolecules due to its capability avoiding the destruction of molecular structure by high energy.However,traditional matrixes usually exhibit strong interference in the low molecular weight range,which greatly limit the application of atmospheric pressure matrix assisted laser ionization source.To solve this problem,a series of matrixes based on new materials have been designed and developed.These new materials could be divided into two categories,ie.new organic matrix and inorganic materials.With the extension of mass range and the sensitivity improvement of target compounds,application of atmospheric pressure matrix assisted laser ionization technique in situ analysis has been greatly expanded.The applications of new matrixes in ambient laser based ionization sources used in the field of food safety were reviewed in this paper,and the future progress was prospected.  
关键词:ambient laser based ionization source;matrix;low molecular weight compound;food safety
摘要:Ambient ionization mass spectrometry plays a pivotal role in the analysis of complex samples owing to the features of no sample pretreatment,easy to use and high efficiency.However,this methodology would result in a simultaneous ionization of sample matrices and target analytes,and the analysis sensitivity of mass spectrometry would be greatly reduced.Solid phase microextraction has been demonstrated to be an effective avenue either to enrich target analytes or to remove matrices from complex samples prior to mass spectrometric analysis,which significantly improves the limit-of-detection of determined compounds.In this work,recent advances in solid phase microextraction techniques,either being coupled directly to ambient ionization sources or capable of in situ ionization of target analytes,are reviewed,and their principles and applications to the analysis of complex samples are summarized.Moreover,the perspectives of solid phase microextraction direct mass spectrometric analysis have been exemplified based on the current development.  
摘要:Vacuum ultraviolet photo ionization(VUV-PI) is a universal soft ionization source for mass spectrometry(MS).The VUV-PI-MS is quite suitable for on line rapid analysis as its mass spectrum is free of fragment ion interference,easy to be interpreted and high sensitive.According to different analytes,VUV-PI could be used in single photon ionization mode or chemical ionization mode achieved by dopant,which could be used for gas,liquid and solid sample analysis,as well as for imaging analysis.The ionization principle of the VUV-PI and the current type of vacuum ultraviolet light source are firstly introduced in this article,then the factors affecting the sensitivity of photo ionization MS and its technical improvement measures are analyzed,and finally,the applications of VUV-PI-MS technology in environmental analysis,chemical products on line analysis,national safety analysis and related application research in biomedical analysis are also presented.In the conclusion,the advantages and disadvantages of VUV-PI are summarized,and the perspectives on developments of performance and applications of VUV-PI technique are looked forward to.  
摘要:Ambient ionization mass spectrometry(AIMS) is a mass spectrometry technology which could be used to analyze target analytes in samples under atmospheric pressure without or with simple sample pretreatment.With the advantages of simplicity,rapidness,non destructiveness and wide application range,it is widely used in forensic toxicological analysis.This article gives a brief overview on the ambient ionization(AI) technique,and the samples are divided into two types:in vivo test materials and in vitro test materials.The application of AIMS in the poison analysis of different types of test materials is summarized,and its application direction in forensic toxicological analysis is prospected.  
关键词:ambient ionization mass spectrometry(AIMS);mass spectrometry;forensic toxicological analysis
摘要:Ambient ionization mass spectrometry(AI-MS) is a kind of novel MS technique,which is performed under ambient conditions without or with few sample pretreatment procedures.In recent years,the development and application of AI-MS technique have attracted increasing attention owing to its advantages,such as real-time,simplicity,rapidness and high throughput.The technical classification and principle characteristics of AI-MS and its application in microbiology research are summarized in this review,and the applications of AI-MS in the identification and typing of bacterial species,bacterial metabolite analysis and biofilm analysis,mass spectrometry imaging,etc.are mainly introduced.So far,ambient ionization combined with portable MS has been more and more widely used,which is anticipated to become a new hot spot in the field of mass spectrometry.  
摘要:Native mass spectrometry has become one of the important tools for characterizing protein structures.Compared with traditional electrospray emitter(ESI emitter),submicron electrospray emitters have various characteristics such as changing the charge state distribution of ions and ion desalting,which could be directly used to analyze the protein structures in the physiological environment.In this review,the characteristics and applications of submicron electrospray emitters in native mass spectrometry analysis are discussed and summarized,and their future developments are also envisioned.  
关键词:submicron electrospray emitters;charge state distribution;ion desalting;native mass spectrometry
摘要:Direct analysis in real time(DART) as an ambient ionization technique has been developed rapidly in recent years.DART combined with mass spectrometry(DART-MS) has become a popular analytical technique,and has been widely used in the field of forensic science,including food safety,explosive detection,toxicological analysis,drug analysis and pharmaceutical analysis,etc.Although conventional detection methods for pesticides have been very common,the introduction of ambient ionization-mass spectrometry can not only broaden the detection range,but also shorten the detection time.The working principle and conditions optimization of DART-MS and its applications in pesticides detection are reviewed in this article.Finally,the application of DART-MS in pesticide detection is briefly prospected.  
关键词:ambient ionization;direct analysis in real time mass spectrometry;pesticide
摘要:The blood's metabolism could be used to provide a precise evaluation on the post surgery physiological status,which poses an urgent technical demand for a point of care test for global metabolomic profiling.Therefore,the practical value of conductive polymer spray ionization mass spectrometry(CPSI-MS) in the multiplex monitoring of endogenous metabolites in a trace volume of whole blood was presented in this paper.The fabricated conductive polymer was composed of carbon nanotube(CNT) and polymethyl methacrylate(PMMA).After applying a high voltage of 4.5 kV for generating charged droplet spray,trace volume of extraction solvent(methanol-H2O,1∶1,5 μL) was enough to extract,desorb and ionize over 600 endogenous metabolites and lipids in the only 1 μL of diluted dried blood spot deposited on the tip,covering more than 20 fundamental metabolism pathways including the energy metabolism,amino acids metabolism,nucleotides metabolism,and lipids metabolism,etc.To give a proof of concept illustration,the C57BL/6 mice experiencing the hepatectomy were selected as the model objects.The individual differences in physiological recovery were precisely characterized by capturing hundreds of metabolites changes with a period of 48 h.Finally,a panel of metabolites mainly in the Krebs cycle,arginine metabolism,glycerolipids metabolism,and glycerophosphorylcholine metabolism could give a prognostic reference for the functional recovery of the mice from the hepatectomy.  
关键词:conductive polymer spray ionization(CPSI);point of care test;metabolomic profile;prognostic marker;hepatectomy
摘要:In recent years,fruit juice adulteration has become an increasingly important issue.Rapid evaporative ionization tandem mass spectrometry(REIMS),as a novel method for real time discrimination of samples,could solve this problem without any sample preparation.In this paper,a metabolomics fingerprinting approach for real time authentication of orange,apple and grapefruit juices was developed.A discriminate model established by principal component analysis(PCA) and linear discriminate analysis(LDA) was able to distinguish different types of fruit juice with a correct classification of 9728% in leave 20% out cross validation and a 100% burns correctly identified in real time recognition.Characteristic m/z markers were detected and some of them were identified.Adulterated orange juices with apple and grape juices at different percentages could be well distinguished from the level of 50% down to 10%.Furthermore,the adulterated samples were analyzed by optimized single MS and tandem MS/MS REIMS(REIMS and REIMS/MS).Partial least squares analysis was successfully used to predict the level of the adulterants(both R2 and Q2>082 for all models).REIMS/MS could offer higher prediction accuracy compared with the conventional REIMS.  
关键词:iKnife;rapid evaporative ionization mass spectrometry(REIMS);metabolomics;fruit juice;adulteration;rapid evaporative ionization tandem mass spectrometry(REIMS/MS)
摘要:Spatially resolved metabolomics methods based on mass spectrometry imaging(MSI) technology have become a powerful tool for biological histology,molecular pathological diagnosis of tumor,and new drug efficacy and toxicology research.In this study,air flow assisted desorption electrospray ionization(AFADESI) with positive/negative mode switched scan was developed for MS imaging.With no need to apply high voltage during the ionization process,this method could not only improve the operating safety of ambient ionization,but also efficiently desorb and ionize various endogenous metabolites from biological tissue slices,especially large area whole body animal tissue slices.Furthermore,it could obtain the spatial distribution characteristics of those metabolites including polyamines,amino acids,phospholipids(easy to ionize in positive ion mode),nucleosides and phosphatidylglycerol(easy to ionize in negative ion mode).Through the simultaneous MSI analysis in positive or negative ion mode,the data collection time and the number of sample slices were saved,and the coverage of metabolites was expanded,while more types of metabolites could be detected in single experiment.Therefore,this method has the advantages in the spatially resolved metabolomics research on various tissues and organs of whole body animals,and it is expected to deeply understand the molecular spatial distribution characteristics and molecular mechanisms related to physiology,pathology and pharmacology at the metabolic level.  
摘要:Isocitrate dehydrogenase(IDH) genotype plays a significant role in precise diagnosis of glioma.An air flow assisted desorption electrospray ionization(AFADESI) mass spectrometry(MS) with rapid sample pretreatment using tissue smear instead of tissue cryo section was developed for rapid determination of the gene status of IDH in human glioma.Using intensity ratio of 2 hydroxyglutaric acid to arachidonic acid as an evaluation index,the IDH gene status of glioma tissue could be quickly identified.Quantitative evaluation as well as investigation on the feasibility for ambient mass spectrometry to analyze the metabolites confirmed that the tissue smear method was capable of rapid analysis of metabolites with high simplicity,high repeatability and high coverage.Receiver operating characteristic curve(ROC) demonstrated that the method possessed a strong diagnostic capacity for identifying the gene status of IDH in glioma.Therefore,the developed method could be expected to be a novel technique for precise diagnosis of glioma.  
关键词:ambient mass spectrometry;tissue smear;isocitrate dehydrogenase;metabolite analysis;air flow assisted desorption electrospray ionization mass spectrometry
摘要:Solid and viscous auxiliaries are often used for manufacturing granules,tablets,capsules and ointments in pharmaceutical industry,which emerge in the promising forms to maintain the stability and activity of various drugs by a variety of matrices.Ambient mass spectrometry(MS) with wooden-tip electrospray ionization(ESI) has been successfully developed for direct analysis of raw drug samples.However,matrix effect in such an ambient ESI-MS analysis on solid and viscous drugs has not yet been well understood.In this work,ionization responses to several modes of drugs in various viscous and solid matrices were investigated using a typical wooden-tip ESI-MS.Ionization responses were found to be related to the solubility of solid matrices.Ionic suppression and interference were observed in soluble solid matrices,while significant ionic interference was not generated in insoluble matrices.However,by adding spray solvent,insoluble matrices were changed in a viscous state suppressing spray ionization process.Further investigation revealed that ionization responses to analytes were decreased as a power function(r2>0.95) with the increase of matrix viscosity from 1 cP to 500 cP in this study.Therefore,this study may provide a good understanding for matrix effect and signal response in substrate ESI-MS analysis on solid and viscous samples.  
关键词:matrix effect;solid samples;viscous samples;solid substrate electrospray ionization;ambient mass spectrometry
摘要:In this study,high resolution mass spectrometry(HRMS) was used to study and characterize carboranes under direct analysis in real time(DART) ionization condition.Generally,good MS signals could be obtained in the determination of carboranes in negative ion DART conditions,which might possibly be the reason of boron cage with “electron deficient” property.In the isotope peaks formed by carboranes containing 10 B atoms at high resolution DART mass spectra,the mass peak with the highest relative abundance normally contains 2 10B atoms and 8 11B atoms.Considering both the accurate high resolution m/z data and isotope mass peaks profile analysis is an effective strategy for qualitative analysis and characterization of carboranes.  
关键词:direct analysis in real time(DART);high resolution mass spectrometry;carboranes
摘要:A rapid identification method for camellia oil was established by direct analysis in real time-quadrupole time-of-flight mass spectrometry(DART-QTOF-MS) combined with chemometrics analysis.Camellia oil,rapeseed oil,peanut oil and soybean oil were accurately weighed,respectively.After dilution,each of them were executed a desorption ionization by DART.In the positive ion mode,the MS data were obtained by TOF MS and information dependent acquisition(IDA) mode,and the mass spectra of four edible oils were preliminarily identified.Meanwhile,the models of principal component analysis(PCA) and orthogonal partial least squares discriminant analysis(OPLS-DA) were established by chemometrics to realize the data visualization and the rapid identification and prediction of camellia oil.Results showed that the main contents in the mass spectra were triacylglycerol ammoniated ions [TAG+NH4]+(m/z 850-1 100),diacylglycerol ammoniated ions [DAG+NH4]+(m/z 600-700) and DART source debris ions.There were obvious differences in the mass spectra of the four edible oils.A total of 20 triacylglycerols and 6 diacylglycerols were detected.The chemometrics analysis could be used for accurate identification and prediction of camellia oil,rapeseed oil,peanut oil and soybean oil.This method is feasible for the rapid identification on authenticity of camellia oil with its advantages of simple pretreatment,quick analysis and easy operation.  
关键词:direct analysis in real time;camellia oil;authenticity;chemometrics
摘要:A direct analysis in real time-mass spectrometry(DART-MS) combined with mechanochemical extraction(MCE) was developed for the analysis of polysaccharides.Eight kinds of herbal polysaccharides including Astragalus membranaceus,Tremella fuciformi,Lilium brownii,Poria cocos,Dendrobium chrysotoxum,Dendrobium nobile,Dendrobium officinale and Codonopsis pilosula were investigated.The extraction results were compared among MCE and traditional extraction methods,and the MCE method was validated and systematically optimized.The polysaccharides were separated by size exclusion chromatography,and the molecular weight calibration curves were constructed,from which the extracted polysaccharide molecular weights were estimated.Meanwhile,DART-MS was used to break down the large polysaccharides into fragment ions m/z<350 in seconds.Different herbal polysaccharides produced characteristic ions which could be used for the efficient identification and differentiation of polysaccharide species.The method,with the characteristics of simplicity,rapidness and no need of sample pre digestion,is a powerful tool for the direct acquirement of distinguished fingerprints from large and complex polysaccharides.  
关键词:polysaccharide;mechanochemical extraction;fingerprint spectra;direct analysis in real time-mass spectrometry(DART-MS)