JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY
·
2025
·
IF 3.1
Jin-Hua Liu,Xiao-Dong Deng,Jian-Wei Li,Lan-Ping Feng,Thomas J. Algeo
The rhenium–osmium (Re–Os) isotopic system has emerged as a widely utilized tool in cosmochemistry and high-temperature geochemical studies. A critical prerequisite for high-precision Os isotope analysis via Negative Thermal Ionization Mass Spectrometry (N-TIMS) involves achieving complete isotopic equilibrium between the sample and spike through the isotope dilution technique. In this study, we present an innovative technique to address valence state disparities in Os species within mixed solutions, thereby enabling effective isotopic equilibration through a chemical reducing reaction with a strong reductant under ambient conditions. Experimental results demonstrate that a solution containing 0.05 mol L−1 hydroxylamine hydrochloride (NH2OH·HCl) coupled with 0.01 mol L−1 HBr effectively stabilizes a nanogram-level Os mass. Systematic optimization of reductant concentration and sample-to-reductant ratio yielded a mean 190Os/188Os value of 1.2280 ± 0.0006 (2s, n = 18) for a mixed Os spike solution, closely aligned with the recommended value of 1.2278 ± 0.0003 (2s, n = 12) obtained through the conventional Carius tube method. Controlled comparative experiments revealed critical considerations for method implementation: (1) a freshly prepared reductant must be employed immediately to ensure reagent efficacy, and (2) precise absolute volume control of the reductant solution is essential to mitigate potential losses of volatile OsO4 linked to extended decomposition times. This novel approach successfully achieves isotopic equilibration between sample–spike and inter-spike components under ambient conditions, offering significant analytical advantages over traditional methods. The validity of the proposed approach was demonstrated by analyzing reference material WMS-1a yielding a 187Os/188Os value of 0.1665 ± 0.0006 (2s, n = 5), which agrees within uncertainty with the established value of 0.1664 ± 0.0003 (2s, n = 5) obtained via the Carius tube method. The protocol enhances operational efficiency by reducing equilibration time and explosive risk, and decreases procedural Os blanks via reducing material and reagent consumption. The combined improvements in precision, cost-effectiveness, and methodological flexibility position this technique as a valuable advancement in Os isotope geochemistry.
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GEOSTANDARDS AND GEOANALYTICAL RESEARCH
·
2013
·Vol. 38
·期 1
·37-50
·
IF 2.77
Jie Li,Xiao-Ying Jiang,Ji-Feng Xu,Li-Feng Zhong,Xuan-Ce Wang,Gui-Qin Wang,Pei-Pei Zhao
en This link goes to a English section fr This link goes to a French section We report an improved procedure for the determination of the platinum-group elements (PGE) and Re, and Os isotopes from a single sample aliquot by isotope dilution (ID) using inductively coupled plasma-mass spectrometry (ICP-MS) and negative thermal ionisation mass spectrometry (N-TIMS), respectively. A two-stage column method was used to purify PGE-Re from their sample matrix and interfering elements (e.g., Mo, Zr and Hf) after Os had been separated by CCl 4 solvent extraction. The first column separation step used cation exchange resin (AG50W-X8) to concentrate PGE-Re and some potential interfering elements (e.g., Mo, Zr and Hf). In the second step, N -benzoyl- N -phenylhydroxylamine (BPHA) extraction resin was used to separate PGE-Re from the remaining interfering elements, which all remained strongly absorbed to the resin. The method was used to determine the PGE and rhenium, and Os isotope ratios in a range of geochemical reference materials (TDB-1, WGB-1, BHVO-2 and UB-N). The obtained results agree well with those previously published. This new method enables PGE-Re abundances and Os isotopic ratios to be determined on the same sample digestion, and circumvents the problems created by sample heterogeneity when comparing PGE and Re-Os isotope data. en This link goes to a English section fr This link goes to a French section Nous décrivons une procédure améliorée pour la détermination des abondances des éléments du groupe du platine (EGP), du Re et des isotopes de l'Os à partir d'un même aliquot d'échantillon par dilution isotopique (ID) en utilisant respectivement la spectrométrie de masse à source plasma (ICP-MS) et la spectrométrie de masse par ionisation thermique négative (N-TIMS). Une méthode sur colonne en deux étapes a été utilisé pour purifier les EGP et le Re de la matrice de l'échantillon et des éléments interférents (par exemple, Mo, Zr et Hf) et ceci après que l'Os ait été séparé par extraction par solvant CCl 4 . La première étape de séparation sur colonne utilise une résine échangeuse de cations (AG50W-X8) pour concentrer les EGP et le Re et certains éléments interférents potentiels (par exemple, Mo, Zr et Hf). Au cours de la seconde étape, la résine d'extraction N-benzoyl-N-phénylhydroxylamine (BPHA) a été utilisée pour séparer les EGP et le Re des éléments interférents restants, qui sont tous fortement absorbé par cette résine. La méthode a été utilisée pour déterminer les concentrations en PGE et Re, et les rapports isotopiques de l'Os dans une gamme de matériaux de référence géochimiques (TDB-1, WGB-1, BHVO-2 et UB-N). Les résultats obtenus sont en bon accord avec ceux publiés antérieurement. Cette nouvelle méthode permet la détermination des abondances en PGE et Re et des rapports isotopiques de l'Os sur la même portion d'échantillon digérée, et contourne ainsi les problèmes liés à l'hétérogénéité des échantillons lorsqu'on compare les données élémentaires des EGP et les données isotopiques Re-Os.
研究领域:
地球化学
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分析化学
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ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Shao-Bin He,Quan-Quan Zhuang,Liu Yang,Mei-Ying Lin,Ye Kuang,Hua-Ping Peng,Hao-Hua Deng,Xing-Hua Xia,Wei Chen
A visual assay for the detection of heparinase was developed on the basis of a ternary system of Hg2+–heparin–osmium nanoparticles (OsNPs). First, heparin-capped OsNPs (heparin–OsNPs) were synthesized by a facile reduction method using heparin as the protecting/stabilizing agent. The oxidase-like activity of heparin–OsNPs, however, turned out to be low, which somewhat limits their application. We discovered that Hg2+ can significantly/specifically boost the oxidase-like activity of heparin–OsNPs via electrostatic interaction. The oxidase-like activity of heparin–OsNPs toward the oxidation of the substrate, 3,3′,5,5′-tetramethylbenzidine, by dissolved O2 was found to increase by 76-fold in the presence of Hg2+. More significantly, heparin in heparin–OsNPs could be specifically hydrolyzed into small fragments in the presence of heparinase, which resulted in the weakening of the oxidase-like activity of Hg2+/heparin–OsNPs. On the basis of these findings, a linear response of the sensor for heparinase was obtained in the range 20–1000 μg/L with a low detection limit (15 μg/L), which is comparable to those of other reported sensors. Further, the colorimetric sensor was employed for the detection of heparinase in human serum samples with satisfactory results. We speculate that combining such surface modification of the osmium nanozyme with a sensing element could be an interesting direction for promoting nanozyme research in medical diagnosis.
研究领域:
生物化学
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医学诊断
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纳米生物学
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Guo Xiaotian,Gao Rui-Ting,Ren Shijie,Nguyen Nhat Truong,Chen Haojie,Wu Limin,Wang Lei
Photoelectrochemical production of ammonia usually suffers from a low solar-to-ammonia efficiency and a high overpotential, which influences the bias-free operation of sustainable photoelectrochemistry. Herein, we realize solar-driven ammonia production from waste nitrate by constructing copper-osmium catalysts deposited on the Sb 2 (S,Se) 3 semiconductor, enabling optimized photo-carrier transport pathways and a beneficial co-adsorption configuration of *NO 3 -H 2 O moieties. The photocathode reaches a photocurrent density of 5.6 mA cm −2 at 0 V RHE with a low onset potential of 0.86 V RHE and a Faradaic efficiency of 96.98% at 0.6 V RHE under AM 1.5 G illumination. We further employ glycerol oxidation reaction on ruthenium doped bismuth oxide catalyst decorated on titanium oxide photoanode, requiring an onset potential of 0.3 V RHE to enable bias-free operation. The unbiased photoelectrochemical system shows Faradaic efficiencies of over 97% for ammonia products and above 77% for glycerol oxidation product under AM 1.5 G illumination. The large-sized photoelectrodes maintain a stability for 24 h without noticeable degradation. Our works indicate that unassisted and stable PEC ammonia production is feasible with in situ glycerol valorization using the photoanode and photocathode.
研究领域:
材料科学
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化学工程
·
能源技术
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 31
·11763-11771
·
IF 4.052
Yaxiong Wei,Min Zheng,Lin Chen,Xiaoguo Zhou,Shilin Liu
Three Os(II) complexes were synthesized with ligands 2,2′-dipyridyl (dipy), 1,10-phenanthroline monohydrate (phen), and 4,7-diphenyl-1,10-phenanthroline (diphen), and applied as triplet photosensitizers for triplet–triplet annihilation (TTA) fluorescence upconversion. The strong spin-orbital coupling made direct spin-forbidden transition of S0–T1 feasible. Lifetimes of the lowest triplet state of these complexes were determined to be 107 ns, 373 ns, and 386 ns for Os-dipy, Os-phen, and Os-diphen, respectively, using nanosecond transient absorption spectra. From steady-state phosphorescence emission spectra, energies of the triplet states were derived to be 1.75 eV, 1.80 eV, and 1.74 eV for Os-dipy, Os-phen, and Os-diphen, respectively. Using these photosensitizers, strong upconverted fluorescence of the triplet acceptors, 9,10-diphenylanthracene (DPA), perylene, and 9,10-bis(phenethynyl) anthracene (BPEA), was observed in the visible to violet range. In particular, fluorescence emission with the largest anti-Stokes shift of 1.14 eV was observed for the Os-phen/DPA system, and the upconverted quantum yield was determined as 5.9% in deoxygenated dichloroethane. Additionally, upconversion was determined in air using mixtures of dichloroethane and DMSO solvents, and the maximal quantum yield was measured to be 4.5% for Os-phen/DPA.
研究领域:
化学
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材料科学
·
光物理学
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Qing Yang,Hanjiao Chen,Jing Hu,Ke Huang,Xiandeng Hou
Efficient simultaneous photochemical vapor generation (PVG) of ruthenium (Ru) and osmium (Os) in the medium of formic acid was demonstrated. A flow-through photoreactor hyphenated to an inductively coupled plasma-mass spectrometer (ICP-MS) was used for the PVG and subsequent detection of the two elements. A similar synergistic enhancement from cobalt and cadmium ions on the PVG efficiency of both Ru and Os was discovered. Following the critical evaluation of the impacts of various transition metal ions, the concentrations of formic acid, cobalt, and cadmium ions, the flow rate of carrier gas, and the UV irradiation time, impressive limits of detection (LODs) of 5 and 0.5 ng L–1 were achieved for Ru and Os, respectively. The accuracy of the proposed PVG-ICP-MS method was validated by the analysis of several water samples with desirable spike recoveries obtained. Furthermore, the volatile compounds of Ru were directed and cryogenically trapped in acetonitrile and generation of carbonyls of Ru was verified by high-resolution electrospray ionization-mass spectra (ESI-MS).
研究领域:
分析化学
·
环境科学
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ACS Applied Bio Materials
·
2025
·
IF 4.7
Ziyu Zhou,Shuo Li,Xiuqian Ding,Kun Zhang,Jie Zhou,Xin Zhou
Photodynamic therapy (PDT) has been demonstrated to be an effective tool for cancer treatment. Seeking organelle-targeting photosensitizers (PSs) with robust reactive oxygen species (ROS) production is extremely in demand. Herein, we propose an aggregation-induced photosensitization strategy for effective PDT with osmium complexes. We designed and synthesized three osmium complexes (Os-Me, Os-tBu, and Os-Nonly) with ligands of different alkyl chains. In phosphate-buffered saline solution, the complex Os-Nonly formed a spherical aggregate with diameters of around 220 nm. The results from ROS assays indicate that Os-Nonly showed the highest efficiency in generating superoxide anions and singlet oxygen, demonstrating its role as a type I/II photosensitizer. Additionally, Os-Nonly specifically targeted lysosomes in 4T1 and MCF-7 cells, producing ROS in a sustained and efficient manner with high phototoxicity (IC50 = 6.999 μM in MCF-7 cells), thereby inducing cancer cell death. In 4T1-tumor-bearing mice models, Os-Nonly effectively inhibited tumor growth with a minimal impact on normal organs.
研究领域:
生物化学
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药理学
·
肿瘤学
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RSC Advances
·
2024
·Vol. 14
·期 14
·9996-10003
·
IF 3.9
Zijie Wei,Cuifeng Jiang,Jinshan Wang,Yue Chen
Metal organic framework (MOF)-derived nanostructures display remarkable characteristics and have broad application potential. Os@ZIF-8 nanocomposites were prepared by a depositional method. The Os nanoparticles distributed on the surface of ZIF-8. The nanocomposites displayed enhanced peroxidase-like activity with smaller Km for both 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2 compared to Os NPs due to the confinement effect and large surface area that ZIF-8 provided. From the average reaction rate constants obtained from three different temperatures, the activation energy values were determined. The kinetic data indicated that the Os@ZIF-8 NCs are catalytically more active than Os NPs. In addition, quantitative measurement of Hg2+ was performed based on the formation of Os–Hg alloy. Os@ZIF-8 NCs had a wide detection range between 0 μM and 71.43 μM for Hg2+ with a limit of detection (LOD) of 2.29 μM. Using a MOF with a large surface area to load Os nanoparticles to achieve enhanced nanozyme activity is the novelty of this work.
研究领域:
材料科学
·
生物化学
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ACS Nano
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2024
·
IF 15.8
P Prabhu,Viet-Hung Do,Takefumi Yoshida,Yingtang Zhou,Hiroko Ariga-Miwa,Takuma Kaneko,Tomoya Uruga,Yasuhiro Iwasawa,Jong-Min Lee
Highly efficient, cost-effective, and durable electrocatalysts, capable of accelerating sluggish reaction kinetics and attaining high performance, are essential for developing sustainable energy technologies but remain a great challenge. Here, we leverage a facile heterostructure design strategy to construct atomically thin Os@Pd metallenes, with atomic-scale Os nanoclusters of varying geometries confined on the surface layer of the Pd lattice, which exhibit excellent bifunctional properties for catalyzing both hydrogen evolution (HER) and oxygen reduction reactions (ORR). Importantly, Os5%@Pd metallenes manifest a low η10 overpotential of only 11 mV in 1.0 M KOH electrolyte (HER) as well as a highly positive E1/2 potential of 0.92 V in 0.1 M KOH (ORR), along with superior mass activities and electrochemical durability. Theoretical investigations reveal that the strong electron redistribution between Os and Pd elements renders a precise fine-tuning of respective d-band centers, thereby guiding adsorption of hydrogen and oxygen intermediates with an appropriate binding energy for the optimal HER and ORR.
研究领域:
材料科学
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电催化
·
能源技术
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2025
·Vol. 122
·期 27
·e2426207122
·
IF 9.1
Wendan Xue,Qixing Zhou,Pengfei Wang,Sijin Zuo,Fengxiang Li,Jiwei Jiang,Fan Mo,Chuan Yin,Gaolei Liu,Zhan Ban,Yuanyuan Wei,Wen An,Xiulin Huang,Hui Wang,Sihui Zhan
Osmium (Os)-based catalysts, recognized for their unique chemical and electronic properties along with cost-effectiveness, hold great potential for the hydrogen evolution reaction (HER). However, their practical application has long been limited because pure Os exhibits excessively strong adsorption of intermediates and suffers from stability issues. Herein, we report the development of a highly stable catalyst achieved by implanting the sulfur (S) atom into the matrix, facilitating the transformation of Os nanocrystals into Os single atoms. The prepared atomically dispersed Os catalyst (Os-SA@SNC) demonstrates outstanding catalytic activity, requiring only a 13 mV overpotential to achieve a current density of 10 mA cm−2 in 1.0 M potassium hydroxide (KOH) solution, as well as the excellent durability. This performance surpasses that of commercial Pt/C and outperforms most of the reported state-of-the-art electrocatalysts. Theoretical simulations clarify the important role of S atoms in promoting the dispersion and diffusion of Os atoms. Moreover, density functional theory calculations indicate that S atoms adjust the local electronic structure of Os active sites, further facilitating the adsorption/dissociation of H2O and optimizing the hydrogen adsorption free energy (ΔG*H), thereby accelerating the kinetics of both the Volmer and Heyrovsky steps in alkaline HER. This work revitalizes Os-based catalysts for energy conversion and paves the way for innovative HER catalyst design and application to contaminated soil/water remediation.
研究领域:
电化学
·
催化
·
纳米材料
·
能量转换
·
密度泛函理论
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MICROCHEMICAL JOURNAL
·
2016
·
IF 2.893
Ying Gao,Shuzhen Li,Hongyan He,Tonglin Li,Ting Yu,Rui Liu,Shijun Ni,Zeming Shi
Accurate analysis of osmium is important in geochemistry and geochronology. The current osmium analytical methods often suffer from low sensitivity, multi-step extraction, high procedural blank, and severe memory effect . In this work, a highly sensitive and simple method for the determination of osmium in natural waters was developed by coupling inductively coupled plasma-mass spectrometry with photochemical vapor generation. The procedural blank is low due to the needlessness of high concentration strong oxidant. What's more, the memory effect was successfully solved by using 5.0% ammonium hydroxide elution instead of using concentrated inorganic acid or oxidant reagent reported before. The influences of the concentration of nitric acid , the flow rate of carrier gas, the photo irradiation time on osmium detection were investigated. Under optimized conditions, the detection limit was 0.8 pg mL − 1 . A precision of 3.2% (RSD, n = 5) was achieved at a concentration of 1 ng mL − 1 . The accuracy is successfully validated in several natural water samples with spike recoveries from 97% to 106%. The proposed method is sensitive, simple, low blank, and memory effect-free, which has a great potential in relevant geochemistry and geochronology study.
研究领域:
地球化学
·
地质年代学
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高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 32
·325401
·
IF 3.953
Ziqiang Wang,Peng Wang,Qiqi Mao,Wenjing Tian,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
The compositional and structural engineering of advanced nanomaterials for hydrogen evolution reaction (HER) is highly necessary for efficient hydrogen production. Herein, PdOs nanospine assemblies (PdOs NAs) with urchin-like structures are fabricated via one-step route using DM-970 and KBr as surfactant agent and capping agent, respectively. Benefiting from electronic effect and multi-branched structure, the PdOs NAs exhibit superior performance for HER in alkaline and neutral solutions, requiring overpotentials of 28 and 35 mV at −10 mA cm−2, respectively, as well as superior long-term stability. This study offers a universal approach for the fabrication of active Pd-based catalysts with multi-branched morphology for efficient water electrolysis and beyond.
研究领域:
材料科学
·
能源化学
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高影响因子
危险品化学品经营许可证（带存储）