Since its inception in 1980, inductively coupled plasma-mass spectrometry (ICP-MS) has developed as the core technology for trace element analysis in modern analytical chemistry. This paper systematically reviews the development history of ICP-MS, covering three dimensions: plasma source, mass analyzer, and the entire instrument, and traces the technical evolution of this technology from the early quadrupole mass spectrometry to high-resolution sector field mass spectrometry, time-of-flight mass spectrometry, and multi-quadrupole ICP-MS/MS. It is pointed out that among numerous technological breakthroughs, the continuous iteration of interference cancellation technology is the key driving force for the development of ICP-MS. From cold plasma technology to quadrupole, hexpole, and octapole collision reaction cells, and then to high-resolution separation technology, the accuracy and sensitivity of trace element analysis in complex matrices have been significantly improved. In terms of analytical capabilities, ICP-MS has surpassed traditional multi-element and isotope analysis, gradually expanding to frontier directions and emerging fields such as speciation analysis and spatial resolution imaging. Single-particle ICP-MS (SP-ICP-MS) enables rapid characterization and quantitative analysis of nanomaterials; single-cell ICP-MS (SC-ICP-MS) provides elemental distribution information at the single-cell level for metallomics research; elemental labeling immunoassay technology opens new avenues for high-throughput multi-index biological detection. Furthermore, mass cytometry integrates the advantages of TOF-ICP-MS with flow cytometry, enabling simultaneous detection of more than 50 protein markers at the single-cell level. In China, ICP-MS has undergone a development process from complete reliance on imports to the gradual rise of domestic instruments. Currently, more than ten domestic enterprises have successfully launched their own brand ICP-MS products. In the future, ICP-MS will continue to provide innovation in the directions of intelligence, automation, and multi-omics integrated analysis, providing more powerful analytical tools for environmental science, life science, materials science, and other fields.

Ideal decomposition of severely overlapped spectra due to limited spectral resolution remains an unsolved puzzle for spectroscopic technologies. Although ultra-high-resolution spectrometers can resolve spectral overlap problems, they often entail high costs and significant signal loss, which naturally leads to relative high limit of detection (LOD). In this work, based on the assumption that the measured spectrum is the convolution of the much less overlapped real plasma emission profile and the spectrometer instrumental response, we propose a center-wavelength coupled with broadening-width-ratio constrained decomposition (CC-BCD) method for severely overlapped peaks from relatively low-resolution spectrometers. More specifically, the method incorporates the extra supporting information (the central wavelengths and the ratio of broadening width of the overlapped peaks obtained from ultra-high-resolution spectra) as hard constraints into the decomposition model, transforming the model from an otherwise underdetermined mathematical fit into a physically guided reconstruction and enabling accurate and stable resolution of severely overlapped peaks. The method was successfully applied for plasma emission technology such as laser-induced breakdown spectroscopy (LIBS) and spark-discharge optical emission spectroscopy (SD-OES). For uranium ores analysis using LIBS, the completely overlapped peaks (U II 385.957 nm and Fe I 385.991 nm) were fully resolved, reducing LOD to 7.3 mg/kg, two orders of magnitude compared with that of using ultra-high-resolution spectrometer and the lowest record ever for ores. For brass sample detection using SD-OES, the severely overlapped peaks (Zn I 328.233 nm and Cu I 328.272 nm) were also resolved, reducing LOD for Zn from 0.39 wt% to 0.11 wt%. The proposed method enables relatively low-resolution spectrometers to achieve high resolution capabilities while retaining the high optical throughput, thereby providing a highly sensitive and low-cost approach for scenarios where the analysis heavily relies on severely overlapped lines, such as ultra-high-sensitivity analysis of uranium in complex matrices.

Mass cytometry (MC), considered the next generation of flow cytometry (FC), uses antibodies tagged with metal isotopes instead of fluorescent molecules for higher-dimensional single cell biomarker assays and can measure more than 50 parameters simultaneously on individual cells. Despite its powerful analytical performance, MC also has limitations in sensitivity and isotope channels using current mass tags. Herein, a new metal tagging strategy was developed to prepare MC mass tags based on apoferritin nanoparticles (AFNPs). For the preparation of AFNPs, rare-earth metals and phosphate ions were sequentially introduced into the cavity of apoferritin by a passive diffusion method to form a metal-phosphate core inside the apoferritin nanocages. The N-hydroxysuccinimide polyethylene glycol (MW = 1000, n = 22) maleimide (NHS-PEG22-MAL) linker was used to link the AFNPs and antibodies to prepare Ab-NP conjugates. The AFNPs have low nonspecific binding to cells, thus resulting in a low background signal for the MC assay. Under optimized conditions, each apoferritin can load an average of 300-800 rare-earth metal atoms, and AFNP tags have more than twice the sensitivity compared with metal-chelating polymer (MCP) tags. Multiparameter assays for the cellular subset analysis of human peripheral blood mononuclear cells (PBMCs) showed good agreement between FC and MC assays by using our AFNP tags. The study presents a new strategy for preparing MC mass tags that are chelator-independent and have multiple staining capabilities, low nonspecific binding, and high sensitivity. The developed AFNP tags are expected to promote the development of MC technology.

Mass cytometry is considered the second generation of flow cytometry technology, which uses metal-labeled antibodies instead of traditional fluorescent antibodies and can measure much more markers from a single cell simultaneously. However, due to frequent clogging of the capillary and nebulizer, it is still a complicated task to perform the sample introduction smoothly for a long-term determination. Herein, a plug-and-play sample introduction device for mass cytometry analysis was developed based on a gas-driven flow focusing protocol. The device is integrated with a virtual hole to generate liquid jet and omit a conventional nebulizer. Single-cell monodispersion can be achieved by liquid jet breakup instead of the commonly used nebulization by the Venturi effect, thus avoiding clogging of thin central capillary. The device has high universality and compatibility and can be plug-and-play on a mass cytometry instrument or common inductively coupled plasma mass spectrometry for single-cell or single-particle determination. High-speed microscopy imaging was used to capture and study the dynamic processes of monodispersion on microsphere suspensions achieved by the device. We also compared the analysis capabilities when using the device and a conventional nebulizer in mass cytometry analysis of four element calibration beads and cell samples. The results obtained by using the flow focusing device and the conventional nebulizer show great consistency, which means the device has no negative impact on the detection performance of mass cytometry and single-cell/particle monodispersion can be achieved without clogging.

Single-atom catalysts (SACs) with electron-rich active sites show high catalytic activity in selective hydrogenation reactions, however, noble metal based SACs are prone to overhydrogenation in selective hydrogenation reactions due to their high dihydrogen dissociation reactivity, resulting in low selectivity of the desired product. Herein, we first report that the Pd SACs supported on TiO2/CNT heterojunction nanocomposite (Pd1Cl1-TiO2/CNT) are successfully prepared by a ball milling combined with acid washing method, wherein the electronic structure of Pd single atoms is synergistically modulated by the heterojunction interface and axial Cl atom coordination, forming a Pd-O4Cl1 structure. As a result, the Pd1Cl1-TiO2/CNT catalyst shows excellent catalytic performance for the selective hydrogenation of cinnamaldehyde (CAL) to hydrocinnamaldehyde (HCAL) under 80 degrees C for 120 min, with a turnover frequency (TOF) of 13.6 min(-1) and a selectivity of 96.7 % at 99.3 % conversion, both much higher than those of SACs with only heterojunction or Cl-axial coordination, surpassing most previously reported Pd-based catalysts. The density functional theory (DFT) calculations show that the excellent catalytic activity is attributed to the interfacial electronic effect of Pd species induced by the heterojunction interface and axially coordinated Cl atoms, which enhances the adsorption of CAL on the Pd-O4Cl1 structure and the desorption of HCAL to inhibit the overhydrogenation. This work provides a new way for the electronic structure modulation of noble metal based SACs for the highly-efficient selective hydrogenation of unsaturated aldehydes.

Materials are the foundation of the manufacturing industry, and high-end materials are one of the most important keys in the upgrading of the manufacturing industry. The key high-end new materials are the cornerstone and forerunner of the development of high-tech industry in the future. The purification of materials has great influence on technology and manufacturing industry, which is the inevitable trend of material development. Therefore, this review discussed the application prospect, significance, development trend and main purity analysis methods of high purity materials. The further development of high technology largely depends on the availability of high purity materials of new functional devices. The further purification of materials has been regarded as an important strategic technology reserve for now days and future in semiconductor, aerospace, new energy, medical devices and other fields. The purity analysis and characterization of high-purity materials is an important step in their purification process, which is crucial for the study of material properties and process improvement. The characteristics of different solid sample analysis techniques such as neutron activation, residual resistivity, emission spectrometry, inductively coupled plasma mass spectrometry, spark source mass spectrometry, glow discharge mass spectrometry and secondary ion mass spectrometry are discussed in this paper. In the absence of high purity standard reference materials, it will be one of the important directions in the development of solid sample analysis technology to study the traceability and quantification factors of various physical phenomena, material properties and matrix effects in the analysis process.

Minimizing sample damage is crucial in laser-induced breakdown spectroscopy (LIBS) for applications involving valuable samples and elemental mapping. In this study, we introduced a low-power atmospheric pressure plasma jet (APPJ) to reduce sample damage by obtaining LIBS signals at significantly lower laser fluences. The proposed technique, APPJ-assisted LIBS (APPJ-LIBS), utilized an argon APPJ to provide seed electrons and enhance the excitation. The APPJ was generated by a 10 kHz alternating current power supply and made contact with the surface of a brass sample at a 30° angle. An infrared nanosecond Nd:YAG laser was focused onto the contacting zone, allowing the resulting laser-induced plasma to evolve within the surrounding APPJ and produce optical emission. The optimized APPJ-LIBS system reduced the laser fluence threshold for spectral detection of the brass sample by 97 %, from 1.43 J/cm2 to 0.05 J/cm2, which represented the lowest laser fluence threshold reported in LIBS studies on copper-based materials. Micrographs of the sample surface showed no visible damage after the APPJ-LIBS measurement at a near-threshold laser fluence and an APPJ input power as low as 6.0 W. Furthermore, gated images showed the plasma evolution in APPJ-LIBS and confirmed the excitation capability of the APPJ for the laser-ablated materials.

Inductively coupled plasma mass spectrometry (ICP-MS) has emerged as a potential analytical platform for clinical detection of biomarkers based on element labeling strategy. However, it is challenging to achieve the routine analysis in clinical laboratory due to the platform's low throughput, low degree of automation, and lack of supporting reagents. Here, we developed a multiplex, high-throughput and automatic immunoassay platform based on rare earth elements (REEs) labeling strategy coupled with ICP-MS detection. On the platform, washing, sampling, rapid uptake and detecting were all automated after manually adding samples. The total time of the entire process can be completed in 40 min. To verify the analytical performance of the platform, the lung cancer five-index immunoassay kits of CEA, CYFRA21-1, NSE, SCC and ProGRP were used as a model. All analytical properties including detection limits, linear range, accuracy, precision, and anti-interference meet the needs of clinical detection. Besides, 350 clinical serum samples were used to validate the platform's potential for clinical application. The developed MSbased immunoassay platform will play an important role for clinical multiplex detection in the fields of cancer, cytokines, and autoimmunity.

Arsenic (As) contamination in drinking water is a global public health problem. Epidemiological studies have shown that selenium (Se) deficiency is associated with an increasing risk of arsenism. However, the association between Se status and As retention in erythrocytes and mechanisms underlying this association have not been fully investigated. In the present study, a total of 165 eligible subjects were recruited and As was found to accumulate in blood mainly by retention in erythrocytes. Retention of As in erythrocytes was negatively correlated with Se status, antioxidant parameters related to Se and As methylation capacity, but positively correlated with the protein-binding capacity of As. Additionally, erythrocytes isolated from subjects with low Se status exhibited cellular damage along with lower protein levels of CD47, which could be aggravated by hydrogen peroxide treatment. Consistent with the human study, the erythrocytes from mice with sub-chronic As exposure exhibited similar cellular damage and shown to be phagocytosed by splenic macrophages, and these effects were mitigated by dietary Se supplementation. Furthermore, hydrogen peroxide treatment induced excessive phagocytosis of erythrocytes with As exposure by splenic macrophages, while co-treating erythrocytes with the reducing agent, N-Acetyl-l-cysteine, mitigated this excessive erythrophagocytosis. Hyperactivation of the NFκB pathway was also detected in splenic macrophages after excessive erythrophagocytosis. In conclusion, this study found that low Se status involving impaired redox homeostasis increased As retention in erythrocytes, which were subsequently phagocytosed by splenic macrophages and led to an increased inflammatory status of splenic macrophages. These findings provide insight into physiological features of arsenism related to Se status and redox homeostasis.

分别用β射线法与重量法对低浓度颗粒物进行测量数据对比分析,测量数据表明β射线法与重量法线性相关强(r>99％);在此基础上,β射线法测量数据的准确度与重复性优于重量法.

Intermediates in the gas-phase reaction of diatomic [TaO]+ with CH4 to generate ethane and ethylene have been explored using ICP-MS/MS complemented by high-level quantum chemical calculations. [TaOH]+, [TaOCH2]+, [TaOC2H6]+and [TaOC2H4]+ were identified and the formation pathways of them were discussed, revealing the mechanistic scenario for this oxidative coupling of methane to the C2 hydrocarbons process.

对细菌特征蛋白和核酸进行高通量定量分析,有助于快速鉴定细菌种群及其功能研究.近年来,结合元素标记策略的电感耦合等离子体质谱(IC P-M S)在细菌蛋白和核酸检测中的应用受到关注.IC P-M S检测蛋白质、核酸等生物分子时,具有灵敏度高、线性范围宽、生物基体干扰小等优点,适用于细菌多组分定量分析.本文综述了细菌不同特征物质作为目标待测物的IC P-M S分析方法,并对其发展方向进行了展望,希望为细菌分析方法的研究提供参考.

In this study, a new immunoassay for the simultaneous determination of pepsinogen I (PGI) and pepsinogen II (PGII) in serum based on element labeling strategy coupled with inductively coupled plasma mass spectrometry (ICP‐MS) detection was proposed.

建立了常压磷酸消解-电感耦合等离子体发射光谱法(ICP-OES)测定钕掺杂钇铝石榴石中Al、Y、Nd元素含量的分析方法.考察了基体元素对掺杂元素测定的干扰情况,实验结果表明Al、Y和Nd的线性关系良好,线性相关系数R均为0.9999,方法检出限分别为0.0032％、0.0004％ 和0.0039％,测定结果的相对标准偏差分别为1.18％、0.94％ 和1.08％,加标回收率在93.3～102.9％ 之间.该方法样品前处理简单、耗时短,适用于Nd:YAG中元素的定量分析.

A multiplex bacterial assay method that combines S1 nuclease pretreatment and ICP-MS-based elemental labels is presented in this work. Six intestinal related bacteria were identified at the species level and quantified simultaneously without isolation culturing. This method could be extended to assay a mixed bacterial community for point-of-care diagnosis.

The Ru+/Ir+ ion-catalyzed reactions of ethanol conversion to butanol have been studied by ICP-MS/MS.

Ethanol to butanol (ETB) process is an attractive route to upgrade abundant substrate into a product with superior properties in energy industry. For the mechanism research, the detection of intermediates is vital. In this paper, intermediates in ETB reaction catalyzed by monoxide ions [ZrO]+/[CeO]+/[TiO]+ were investigated by inductively coupled plasma tandem mass spectrometry (ICP-MS/MS). Some important organic small molecule intermediates, metal-adduct intermediates and their formation pathways were discussed to reveal the reaction mechanism in this research. Isotopic labelling experiments were also designed to ensure the existence of these intermediates.

A new method for chemical vapor generation by hydrogen-containing plasma has been proposed for Se solid sampling.

A portable, miniaturized atomizer-based dielectric barrier discharge (DBD) device was developed for the simultaneous speciation of mercury into inorganic mercury (Hg2+), methylmercury (MeHg), and ethylmercury (EtHg) by HPLC-CVGAFS. The analytical performance as well as the optimum separation and detection conditions of the modified methodology were evaluated. Using the optimized conditions, the minimum quantitative limits obtained were 0.084, 0.086, 0.093 mu g L-1 for Hg2+, MeHg and EtHg, respectively. The relative standard deviations (RSDs, n = 7) from 8 mu g L-1 Hg2+, MeHg, and EtHg were 3.7%, 4.8%, and 3.9%, respectively. In addition, the certified reference material GBW10029 Fish was used to verify the feasibility and potential of the new atomizer for the speciation of Hg on-line and in the field.

Multiplex biomolecular analysis with inductively coupled plasma mass spectrometry (ICP-MS) becomes increasingly important in clinical diagnosis and single cell analysis. However, the sensitivity of ICP-MS-based immunoassay is only comparable or lower than those of fluorescence methods at the present stage. Therefore, designing elemental tags with a large number of metal atoms is necessary to achieve high-sensitive detection. In this work, we proposed a new strategy to build up elemental tag loading with hundreds of rare earth ions by coupling alkyne-DNA chains with rare earth element (REE)-DOTA complexes a click chemistry reaction. There are about 2 orders of magnitude improvement in sensitivity compared with single metal-ion tags. DNA chains with multialkynyl groups were facilely prepared by PCR synthesis. Moreover, the DNA-based elemental tags own excellent water-solubility and biocompatibility. The tags would be potentially applied to mass cytometry and clinical diagnosis.