- 标题
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Development of ZnO Nanoparticles as an Efficient Zn Fertilizer: Using Synchrotron-Based Techniques and Laser Ablation to Examine Elemental Distribution in Wheat Grain
摘要： Zinc (Zn) deficiency is an important problem worldwide, adversely impacting human health. Using a field trial in China, we compared the foliar-application of both ZnO nanoparticles (ZnO-NPs) and ZnSO4 on winter wheat (Triticum aestivum L.) for increasing the Zn concentration within the grain. We also used synchrotron-based X-ray fluorescence microscopy (μ-XRF) and laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) to examine the distribution of Zn within the grain. We found that ZnO-NPs increase the Zn concentration in the wheat grain, increasing from 18 mg·kg-1 in the control up to 40 mg·kg-1 when the ZnO-NPs were applied four times. These grain Zn concentrations in the ZnO-NP-treated grains are similar to those recommended for human consumption. However, the ZnO-NPs were similar in their effectiveness to ZnSO4. When examining trace element distribution in the grain, the trace elements were found to accumulate primarily in the aleurone layer and the crease region across all treatments. Importantly, Zn concentrations in the grain endosperm increased by nearly 30-fold relative to the control, with this markedly increasing Zn within the edible portion. These results demonstrate that ZnO-NPs is a suitable fertilizer for increasing Zn within wheat grain and can potentially be used to improve human nutrition.
关键词： X-ray fluorescence microscopy (μ-XRF),foliar application,wheat,Zn biofortification,laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS),ZnO-NPs
更新于2025-09-19 17:13:59
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Mass Spectrometry Imaging of Triglycerides in Biological Tissues by Laser Desorption Ionization from Silicon Nanopost Arrays
摘要： Mass spectrometry imaging (MSI) is used increasingly to simultaneously detect a broad range of biomolecules, while mapping their spatial distributions within biological tissue sections. Matrix-assisted laser desorption ionization (MALDI) is recognized as the method-of-choice for MSI applications due in part to its broad molecular coverage. In spite of the remarkable advantages offered by MALDI, imaging of neutral lipids, such as triglycerides (TGs), from tissue has remained a significant challenge due to ion suppression of TGs by phospholipids, e.g., phosphatidylcholines (PCs). To help overcome this limitation, silicon nanopost array (NAPA) substrates were introduced to selectively ionize TGs from biological tissue sections. This matrix-free laser desorption ionization (LDI) platform was previously shown to provide enhanced ionization of certain lipid classes, such as hexosylceramides (HexCers) and phosphatidylethanolamines (PEs) from mouse brain tissue. In this work, we present NAPA as an MSI platform offering enhanced ionization efficiency for TGs from biological tissues relative to MALDI, allowing it to serve as a complement to MALDI-MSI. Analysis of a standard lipid mixture containing PC(18:1/18:1) and TG(16:0/16:0/16:0) by LDI from NAPA provided an ~49 and ~227-fold higher signal for TG(16:0/16:0/16:0) relative to MALDI, when analyzed without and with the addition of a sodium acetate, respectively. In contrast, MALDI provided an ~757 and ~295-fold higher signal for PC(18:1/18:1) compared to NAPA, without and with additional Na+. Averaged signal intensities for TGs from MSI of mouse lung and human skin tissues exhibited an ~105 and ~49-fold increase, respectively, with LDI from NAPA compared to MALDI. With respect to PCs, MALDI provided an ~2 and ~19-fold increase in signal intensity for mouse lung and human skin tissues, respectively, when compared to NAPA. The complementary coverage obtained by the two platforms demonstrates the utility of using both techniques to maximize the information obtained from lipid MS or MSI experiments.
关键词： laser desorption ionization,Mass spectrometry imaging,NAPA,nanopost array,lipids,triglycerides
更新于2025-09-19 17:13:59
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An approach to analysis of primary amines by a combination of thin‐layer chromatography and matrix‐assisted laser desorption ionization mass spectrometry in conjunction with post‐chromatographic derivatization
摘要： On-spot derivatization has been suggested for the modification of primary amine containing compounds for their analysis by thin-layer chromatography hyphenated with matrix-assisted laser desorption ionization mass spectrometry. The proposed approach was based on post-chromatographic treatment of separated analytes inside the chromatographic zones on the thin-layer chromatography plates by tris(2,6-dimethoxyphenyl)methilium reagent. The derivatives, containing permanent positive charge, reveal exceptionally intense peaks of their cationic moieties and high signal/noise ratio in mass spectra recorded directly from the plates. The method was tested on a series of aliphatic, aromatic, and amine-containing pharmaceuticals.
关键词： thin-layer chromatography,mass spectrometry,primary amines,matrix-assisted laser desorption/ionization,derivatization
更新于2025-09-19 17:13:59
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Enrichment and Identification of Metallothionein by Functionalized Nano-Magnetic Particles and Matrix Assisted Laser Desorption Ionization Time-of-Flight Mass Spectrometry
摘要： As a low molecular weight protein with the ability of binding metal ions and high inducibility, metallothionein (MT) is often regarded as an important biomarker for assessment of heavy metal pollution in water environment. In the light of that the traditional process of enrichment and identification is time-consuming and complicated, we prepared a core-shell nanoparticle, gold-coated iron oxide nanoparticles (Fe3O4@Au NPs) herein. It possessed the advantages of fast response to magnetic fields and optical properties attributing to Fe3O4 and Au nanoparticles, respectively. The Fe3O4@Au nanoparticles could be used to enrich MT simply through Au–S interaction, and the purified proteins were determined by matrix assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF/MS). The results showed that the Fe3O4@Au nanoparticles could directly enrich MT from complex solutions and the detection limit could be as low as 10 fg mL?1.
关键词： Core-shell structure,Mass spectrometry,Low-abundant,Metallothionein,Gold nanoparticles,Magnetic nanomaterials
更新于2025-09-19 17:13:59
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Iolite Based Bulk Normalization as 100% (m/m) Quantification Strategy for Reduction of Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry Transient Signal
摘要： Iolite package draw more attention in laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) community in recent years due to its powerful data-handling capacity, excellent signal visualization and open source of calculation codes. In this study, the application of Iolite package was investigated for LA-ICP-MS elemental quantification, and a calculation code for the bulk normalization as 100% (m/m) strategy was compiled. We found that the spline interpolation approach was better than that of linear one for the correction of time-dependent instrument drift. BCR-2G as the quality material was used to assess the proposed code, and the results revealed that the code was practical and reliable. The analytical accuracy was influenced by the used calibration materials. TiO2, MgO, K2O and rare earth elements in BCR-2G were slightly off (5%–10%) when NIST SRM 610 as the calibrator. Cr and Mo were higher (10%–30%) than the recommended values when StHs6/80-G was used as the calibrator. The phenomena would be attributed to the matrix effect or the inaccurate values of corresponding calibrators. Three main sources for the LA-ICP-MS combined uncertainty were recognized, including the uncertainty of recommended values of analytes in calibration material, the uncertainty of measured intensity ratios in sample and the error in bulk normalization as 100% (m/m) strategy. A total of 50 elements in CGSG glass reference materials were quantified based on the proposed Iolite code. Major elements (except MnO, CaO and P2O5) matched well with the recommended values with a discrepancy of 5%, and the trace elements (except Cr, Ni, Zn, Ga, Mo and Sb) were agreement with the recommended values in 10%. The dataset reported in this study was helpful for the value certification of CGSG reference materials. Overall, the proposed Iolite code broadened the application of Iolite package in the reduction of LA-ICP-MS transient signal for the elemental determination.
关键词： CGSG reference material,Combined uncertainty,Laser ablation-inductively coupled plasma-mass spectrometry,Iolite package,Bulk normalization as 100% (m/m)
更新于2025-09-19 17:13:59
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The Diagnosis of Sulfated Hemoglobin (SulfHb) Secondary to Sulfur Dioxide Poisoning Using Matrix-Assisted Laser Desorption Time-of-Flight Mass Spectrometry (MALDI-ToF MS)a??A Novel Approach to an Unusual Clinical Problem
摘要： Sulfhemoglobinemia is a rare entity caused by irreversible sulfation of the heme moiety in haemoglobin to form sulfated haemoglobin (SulfHb) and has been caused by H2S arising from certain metabolites of drugs and bacterial infection. Clinical presentation is similar to that of methemoglobin (MetHb). Furthermore, it is often difficult to distinguish between the diagnosis of SulfHb from MetHb in arterial blood gas analysers due to the broad overlap in the optical density (OD) absorption spectra—that of SulfHb swamping the more distinct OD absorption shift seen with MetHb. The presence of SulfHb was suspected in a 73-year-old lady with low oxygen saturation (SaO2 ~75%), central cyanosis, and normal arterial oxygen partial pressure (pO2 ~12 kPa). Repeated arterial blood gas analysis on different systems returned error messages for MetHb quantification. There was an improvement in oxygen saturation and cyanosis after an exchange transfusion. A full OD spectrophotometry (500–700 nm) of the patient’s whole blood was suggestive of the presence of SulfHb, with a minor peak absorption at 620 nm. Matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-ToF MS) was undertaken on whole blood samples from the patient pre- and post-transfusion, alongside normal controls. These demonstrated the presence of SulfHb in the patient’s blood, identifying sulfur, sulfur monoxide, and sulfur dioxide bound to the heme moiety. This gave vital identification as to the cause of Hb sulfation, which was distinct from that previously reported. Levels fell after the exchange transfusion and were completely eradicated after the correct source, an Epsom Salts constipation tonic, was identified. MALDI-ToF mass spectrometry is a new, rapid, specific, and sensitive diagnostic test for rare hematological syndromes such as SulfHb. In addition, it can identify the specific compounds bound to heme. Here, we provide useful diagnostic evidence as to the source of SulfHb, which was via SO2 rather than the previously described H2S.
关键词： SulfHb diagnosis,sulfated haemoglobin,mass spectrometry,MALDI-TOF MS,arterial blood gas analysers,oxygen saturation,MetHb
更新于2025-09-19 17:13:59
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{Nanoa??gold, Iron (III)a??1,3,5a??benzene tricarboxylate Metal Organic Framework (MOF)} nanoa??composite as precursor for Laser Ablation Generation of golda??iron AumFen+/a?? (m = 1a??35, n=1a??5) clusters. Mass spectrometric study
摘要： Gold-iron bimetallic materials have applications in many fields, especially in nanotechnology and biomedicine. The chemistry of iron doped gold clusters is still not fully understood but opens up the possibility of developing new materials, e.g. of gold cages doped with iron atoms. There have been several theoretical studies on these clusters but only a few experimental studies. Laser desorption ionisation (LDI) was used for the generation of Au-Fe bimetallic clusters via laser ablation (337 nm nitrogen laser) of the synthesised nano-composite {nano-gold; Fe(III) 1,3,5-benzene tricarboxylate}, i.e. {AuNPs, Fe-MOF}, while a quadrupole ion trap time of flight mass spectrometer, equipped with a reflectron, was used to acquire mass spectra. A {AuNPs, Fe-MOF} nano-composite was prepared and found suitable for the LDI generation of AumFen clusters. In addition to Aum+/- (m = 1-35) clusters, a series of positively and negatively charged gold-iron AumFen+/- ones were generated. The mass spectra exhibited evidence for the clusters containing up to five iron atoms. In total, 113 binary AumFen+/- clusters (m = 1-35, n =1-5) were identified in the gas phase. A synthesised {AuNPs, Iron (III)-1,3,5-benzene tricarboxylate MOF} nano-composite was found suitable for the generation of many new gold-iron clusters and mass spectrometry was shown to be an efficient technique for the determination of the cluster stoichiometry. A broad series of over 100 bimetallic AumFen clusters, some of them suggested to be gold cages doped with iron atoms (for m = 12 and higher), not only demonstrate a rich and complex chemistry, but also open wide possibilities of biomedical applications.
关键词： nanoparticles,Mass spectrometry,MOF,Gold-iron,Laser desorption ionisation,Clusters,Nano-composite
更新于2025-09-19 17:13:59
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Highly selective and sensitive online measurement of trace exhaled HCN by acetone-assisted negative photoionization time-of-flight mass spectrometry with in-source CID
摘要： Exhaled hydrogen cyanide (HCN) has been extensively investigated as a promising biomarker of the presence of Pseudomonas aeruginosa in the airways of patients with cystic fibrosis (CF) disease. Its concentration profile for exhalation can provide useful information for medical disease diagnosis and therapeutic procedures. However, the complexity of breath gas, like high humidity, carbon dioxide (CO2) and trace organic compounds, usually leads to quantitative error, poor selectivity and sensitivity for HCN with some of existing analytical techniques. In this work, acetone-assisted negative photoionization (AANP) based on a vacuum ultraviolet (VUV) lamp with a time-of-flight mass spectrometer (AANP-TOFMS) was firstly proposed for online measurement of trace HCN in human breath. In-source collision-induced dissociation (CID) was adopted for sensitivity improvement and the signal response of the characteristic ion CN? (m/z 26) was improved by about 24-fold. For accurate and reliable analysis of the exhaled HCN, matrix influences in the human breath including humidity and CO2 were investigated, respectively. A Nafion tube was used for online dehumidification of breath samples. Matrix-adapted calibration in the concentration range of 0.5–50 ppbv with satisfactory dynamic linearity and repeatability was obtained. The limit of quantitation (LOQ) for HCN at 0.5 ppbv was achieved in the presence of 100% relative humidity and 4% CO2. Finally, the method was successfully applied for online determination of human mouth- and nose-exhaled HCN, and the nose-exhaled HCN were proved to be reliable for assessing systemic HCN levels for individuals. The results are encouraging and highlight the potential of AANP-TOFMS with in-source CID as a selective, accurate, sensitive and noninvasive technique for determination of the exhaled HCN for CF clinical diagnosis and HCN poisoning assessment.
关键词： Cystic fibrosis,Acetone-assisted negative photoionization,Hydrogen cyanide,Time-of-flight mass spectrometry,Pseudomonas aeruginosa,In-source collision-induced dissociation
更新于2025-09-19 17:13:59
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Fundamentals and Applications of Fourier Transform Mass Spectrometry || Fourier transform ion cyclotron resonance mass spectrometry and laser: A versatile tool
摘要： The coupling of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) with laser combines the attributes of laser mass spectrometry with the analytical capabilities of a mass spectrometer having high resolution, high mass measurement accuracy, long ion-observation times, and exceptional ion isolation capabilities required for ion-molecule reaction or ion fragmentation studies [1–3]. The laser may be used for different purposes in mass spectrometry. The most standard one is to generate ions from the surface of the laser-irradiated sample. Two regimes have to be considered in respect with the laser fluence (energy deposit per surface unit in J/cm2) or the laser power density also named irradiance (power density deposit per surface unit in W/cm2). At low laser fluence, laser desorption/ionization (LDI) may take place. When the laser fluence increases, the regime of laser–matter interaction is modified and laser ablation (LA) occurs. In both cases, the ionization phenomenon and the transfer of the atoms or molecules to the gas phase are the direct result of the laser matter interaction. LDI and LA are well suited to the analysis of a wide range of organic, inorganic and also biological compounds. For complex matrices, it is important to note that information may be obtained on both organic and inorganic species. This is of first importance for the study of environmental or composite samples for example, in which organics, inorganics and/or polymers are intimately associated.
关键词： laser,Fourier transform ion cyclotron resonance mass spectrometry,laser desorption/ionization,organic compounds,mass spectrometry imaging,inorganic compounds,laser ablation
更新于2025-09-16 10:30:52
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Correlated Secondary Ion Mass Spectrometry-Laser Scanning Confocal Microscopy Imaging for Single Cell-Principles and Applications
摘要： Secondary ion mass spectrometry (SIMS) as a powerful surface analysis technique has been widely applied in semiconductor industry and geology research. Recently, with the development of instrumental technology, SIMS is attracting more and more attention in life sciences. SIMS can provide surface MS spectra, 2D/3D chemical images and depth profiling of substances simultaneously. The minimal lateral resolution of 2D SIMS imaging is 80?100 nm, and the longitudinal resolution of 3D SIMS imaging is about 1–5 nm. However, owing to lack of specific ions to render the structures of organelles, SIMS imaging for single cells still have great challenges. Optical microscopy, in particular laser scanning confocal microscopy (LSCM), has been emerged to be an indispensable technique for single cell imaging and can obtain high spatial 2D/3D imaging to visualize the structures of organelles. Thus, the combinational use of SIMS and LSCM, which takes advantages of SIMS for molecular imaging and LSCM for morphological imaging, has greatly extended the application of SIMS imaging and ensured its accuracy at single cells level, providing novel insights into better understanding of the biological events inside cells. In this review, we focus on the development and application of SIMS imaging and the correlated SIMS and LSCM imaging in the research of cell biology and drug discovery. We anticipate that the combinational use of SIMS and LSCM imaging has promising future in biomedicine and life sciences.
关键词： Cell biology,Single cell imaging,Laser scanning confocal microscopy,Correlated secondary ion mass spectrometry and laser scanning confocal microscopy imaging,Secondary ion mass spectrometry,Review
更新于2025-09-16 10:30:52