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1.
Sci Rep ; 13(1): 17415, 2023 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-37833371

RESUMO

In this study, we present a validated Geant4 Monte Carlo simulation model of the Dingo thermal neutron imaging beamline at the Australian Centre for Neutron Scattering. The model, constructed using CAD drawings of the entire beam transport path and shielding structures, is designed to precisely predict the in-beam neutron field at the position at the sample irradiation stage. The model's performance was assessed by comparing simulation results to various experimental measurements, including planar thermal neutron distribution obtained in-beam using gold foil activation and [Formula: see text]B[Formula: see text]C-coated microdosimeters and the out-of-beam neutron spectra measured with Bonner spheres. The simulation results demonstrated that the predicted neutron fluence at the field's centre is within 8.1% and 2.1% of the gold foil and [Formula: see text]B[Formula: see text]C-coated microdosimeter measurements, respectively. The logarithms of the ratios of average simulated to experimental fluences in the thermal (E[Formula: see text] 0.414 eV), epithermal (0.414 eV < E[Formula: see text] 11.7 keV) and fast (E[Formula: see text] 11.7 keV) spectral regions were approximately - 0.03 to + 0.1, - 0.2 to + 0.15, and - 0.4 to + 0.2, respectively. Furthermore, the predicted thermal, epithermal and fast neutron components in-beam at the sample stage position constituted approximately 18%, 64% and 18% of the total neutron fluence.

2.
Sci Total Environ ; 830: 154706, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35331767

RESUMO

Increasing concentrations of Rare Earth Elements (REE) plus yttrium (REY) are entering the environment due to human activities. The similar chemical behaviour across the whole REY, i.e. the lanthanide series (lanthanum to lutetium) and yttrium, allows their use as tracers, fingerprinting rock-forming processes and fluid-rock interactions in earth science systems. However, their use in fingerprinting waste and particularly low-level radioactive waste has not received much attention, despite the direct use of REE in the nuclear industry and the traditional use of REE as proxies to understand the environmental mobility of the actinide series (actinium to lawrencium). The highly instrumented low-level radioactive waste site at Little Forest (Australia) allows a detailed REY study, investigating interactions with local strata, neighbouring waste forms and shallow groundwater flows. Groundwater samples and solids from cored materials were recovered from 2007 to 2012 from the study site and regional baseline sites in the same geological materials. The REY in water samples were analysed by automated chelation pre-concentration (SeaFast, ESI) followed by ICP-MS determination, while solid samples were analysed using Neutron Activation Analysis (NAA) and X-ray fluorescence scanning (ITRAX). Solid rocks showed no REY departed from typical Upper Crust compositions in either Little Forest or regional background sites. Shallow groundwater from ~4-5 m, at or slightly below waste trench levels, showed water-waste interaction as a marked enrichment, relative to shale-normalised patterns, in samarium, europium and gadolinium, with depleted yttrium. Leachate samples from the neighbouring urban landfill show different REY normalised patterns. REY distribution changes with depth through increased interaction with shales and sandstones. Variations in pH and redox conditions lead to widespread precipitation of Fe-hydroxides, which scavenge REY with differential uptake by precipitating solids, resulting in increases in Y and higher Y/Ho ratio in the groundwater along the flow path. Our study revealed that the Little Forest low-level radioactive waste has a REY fingerprint different to that of groundwater in surrounding land uses. REY can be used to fingerprint diverse waste sources, assess the mobility of lanthanides inferring the mobility of selected actinides, and to trace the fate of REY during groundwater recharge. The approach presented can refine source allocation and trace pollutant mobility in current and legacy urban, mixed and radioactive waste sites around the world.


Assuntos
Água Subterrânea , Metais Terras Raras , Resíduos Radioativos , Poluentes Químicos da Água , Monitoramento Ambiental/métodos , Água Subterrânea/química , Humanos , Metais Terras Raras/análise , Resíduos Radioativos/análise , Água/análise , Poluentes Químicos da Água/análise , Ítrio
3.
J Environ Radioact ; 234: 106627, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-33964669

RESUMO

Data on the uptake of elements and radionuclides by flora from soils in arid environments are underrepresented in international databases, especially when comparing across seasons. This study improved the understanding on the uptake of natural uranium-series radionuclides, as well as more than 30 elements, in a range of Australian native flora species that are internationally representative of an arid/semi-arid zone (e.g. Acacia, Astrebla, Atriplex, and Dodonea). Results indicate that the soil-to-plant uptake ratios were generally higher when compared with international data for grasses and shrubs from more temperate environments. The majority of the elemental concentrations in grasses were higher in winter than in summer and the opposite trend was found in shrubs, which suggests that the season of collection potentially introduces variability in the reported concentration ratios. The data also suggest that grasses, being dominant and widespread species in arid zones, may be effective as a reference organism to ensure comparative assessment across sites of interest. The results of this study will improve the confidence of environmental assessments in arid zones.


Assuntos
Monitoramento de Radiação , Austrália , Radioisótopos , Estações do Ano , Solo
4.
PLoS One ; 14(5): e0216895, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31083691

RESUMO

An evaluation of the geochemical characteristics of 102 storage jar sherds by k0-neutron activation analysis (k0-NAA) from archaeological contexts in Cambodia and reference samples from stoneware production centres in Thailand provides a new perspective on regional and global trade in mainland Southeast Asia. Identification of seven geochemical groups enables distinctions between production centres, and articulation of their role in trade between northern and central Thailand, South China and Cambodia. Storage jars from Thailand and South China are known in archaeological contexts worldwide because of their durability and intrinsic functional and cultural values. Evidenced by a novel application of k0-NAA, analogous stoneware sherds at Longvek connect the Cambodian capital to a global trading network. Additional proof of ceramics from an undocumented Cambodian kiln demonstrates the gradual and complex transition between the Angkorian past and the Early Modern period.


Assuntos
Arqueologia , Cerâmica/história , Comércio/história , Camboja , História do Século XV , História do Século XVI , História do Século XVII , Humanos
5.
Anal Chem ; 89(12): 6314-6317, 2017 06 20.
Artigo em Inglês | MEDLINE | ID: mdl-28590112

RESUMO

The practical realization of the unit of mass is possible by manufacturing a perfect one-kilogram sphere from a 28Si-enriched single crystal. The mass of the sphere can be determined in terms of a fixed value of the Planck constant by counting the number of silicon atoms in the core of the single crystal. To reach the target 2.0 × 10-8 relative standard uncertainty, the mass of the surface layer and the mass deficit due to point defects such as impurities and vacancies must be investigated and corrected for. A sample of a 28Si-enriched single crystal produced to test the possibility of obtaining material at a scale useful to the dissemination of mass standards was measured by instrumental neutron activation analysis to check the purity with respect to a large number of possible contaminant elements. The results collected in a neutron activation experiment performed with the high thermal neutron flux available at the 20 MW OPAL research reactor are described. The data collected in this study showed that the produced material has a purity level never achieved with silicon used to manufacture previous one-kilogram spheres.

6.
Anal Chem ; 89(12): 6726-6730, 2017 06 20.
Artigo em Inglês | MEDLINE | ID: mdl-28514844

RESUMO

The use of new silicon single crystals highly enriched in 28Si recently produced for the upcoming redetermination of the Avogadro constant requires knowledge of their molar masses. The isotopic composition data are collected independently in different laboratories but all using the virtual element technique with multicollector inductively coupled plasma mass spectrometers. In this framework, the comparison of the results with an independent measurement of the amount of at least one of the depleted isotopes is useful to limit hidden systematic errors. To this aim, the 30Si mole fraction of a sample of the new material was measured using a relative measurement protocol based on instrumental neutron activation analysis. The protocol is similar to that previously applied with the AVO28 silicon material used for the last determination of the Avogadro constant value with the exception that unknown and standard samples are not coirradiated. The x(30Si) = 5.701 × 10-7 mol mol-1 estimate is close to the expected one and is given with a standard uncertainty of 8.8 × 10-9 mol mol-1. This value, if adopted, gives a contribution to the relative standard uncertainty of the Avogadro constant of 6.3 × 10-10.

7.
Environ Geochem Health ; 39(3): 549-563, 2017 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-27146864

RESUMO

Mine wastes and tailings are considered hazardous to human health because of their potential to generate large quantities of highly toxic emissions of particulate matter (PM). Human exposure to As and other trace metals in PM may occur via inhalation of airborne particulates or through ingestion of contaminated dust. This study describes a laboratory-based method for extracting PM2.5-10 (coarse) and PM2.5 (fine) particles from As-rich mine waste samples collected from an historical gold mining region in regional, Victoria, Australia. We also report on the trace metal and metalloid content of the coarse and fine fraction, with an emphasis on As as an element of potential concern. Laser diffraction analysis showed that the proportions of coarse and fine particles in the bulk samples ranged between 3.4-26.6 and 0.6-7.6 %, respectively. Arsenic concentrations were greater in the fine fraction (1680-26,100 mg kg-1) compared with the coarse fraction (1210-22,000 mg kg-1), and Co, Fe, Mn, Ni, Sb and Zn were found to be present in the fine fraction at levels around twice those occurring in the coarse. These results are of particular concern given that fine particles can accumulate in the human respiratory system. Our study demonstrates that mine wastes may be an important source of metal-enriched PM for mining communities.


Assuntos
Arsênio/análise , Resíduos Perigosos/análise , Resíduos Industriais/análise , Mineração , Material Particulado/química , Oligoelementos/análise , Poluentes Atmosféricos , Humanos , Laboratórios , Tamanho da Partícula , Vitória
8.
Anal Chem ; 88(13): 6881-8, 2016 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-27282500

RESUMO

At present, counting atoms in a one-kilogram sphere made of (28)Si-enriched silicon allows the determination of the Avogadro constant with the 2.0 × 10(-8) relative standard uncertainty required for the realization of the definition of the new kilogram. With the exception of carbon, oxygen, boron, nitrogen, and hydrogen, the claimed uncertainty is based on the postulation that the silicon material used to manufacture the sphere was above a particular level of purity. Two samples of the silicon were measured using instrumental neutron activation analysis to collect experimental data to test the purity assumption. The results obtained in two experiments carried out using different research reactor neutron sources are reported. The analysis confirmed that the silicon material was of sufficient purity by quantifying the ultratrace concentration of 12 elements and determining the detection limits of another 54 elements.

9.
Environ Geochem Health ; 38(5): 1097-1114, 2016 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-26537592

RESUMO

Abandoned historical gold mining wastes often exist as geographically extensive, unremediated, and poorly contained deposits that contain elevated levels of As and other potentially toxic elements (PTEs). One of the key variables governing human exposure to PTEs in mine waste is particle size. By applying a size-resolved approach to mine waste characterisation, this study reports on the proportions of mine waste relevant to human exposure and mobility, as well as their corresponding PTE concentrations, in four distinct historical mine wastes from the gold province in Central Victoria, Australia. To the best of our knowledge, such a detailed investigation and comparison of historical mining wastes has not been conducted in this mining-affected region. Mass distribution analysis revealed notable proportions of waste material in the readily ingestible size fraction (≤250 µm; 36.1-75.6 %) and the dust size fraction (≤100 µm; 5.9-45.6 %), suggesting a high potential for human exposure and dust mobilisation. Common to all mine waste types were statistically significant inverse trends between particle size and levels of As and Zn. Enrichment of As in the finest investigated size fraction (≤53 µm) is of particular concern as these particles are highly susceptible to long-distance atmospheric transport. Human populations that reside in the prevailing wind direction from a mine waste deposit may be at risk of As exposure via inhalation and/or ingestion pathways. Enrichment of PTEs in the finer size fractions indicates that human health risk assessments based on bulk contaminant concentrations may underestimate potential exposure intensities.


Assuntos
Arsênio/análise , Poluentes Ambientais/análise , Tamanho da Partícula , Monitoramento Ambiental/métodos , Poluentes Ambientais/química , Ouro , Humanos , Resíduos Industriais/análise , Mineração , Medição de Risco , Vitória , Zinco/análise , Zinco/química
10.
Anal Chem ; 87(7): 3699-705, 2015 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-25723904

RESUMO

Instrumental neutron activation analysis with both relative and k0 standardization was used in four experienced laboratories to determine element mass fractions in single-wall carbon nanotube certified reference material (CRM) SWCNT-1. Results obtained were evaluated using the National Institute of Standards and Technology (NIST) "Type B On Bias" approach and yielded consensus values in agreement with National Research Council Canada (NRCC) certified values for Fe, Co, Ni, and Mo and provided mass fraction values for 13 additional elements, namely, Na, Mg, Al, K, Ca, Ti, V, Cr, Mn, Br, La, W, and Au. In addition, prompt γ neutron activation analysis was employed to determine mass fractions of H, B, Co, Ni, and Mo. Results of this work provide a basis for the establishment of reference values of element mass fractions in CRM SWCNT-1, thus expanding its usability for more accurate characterization and benchmarking of similar nanotechnology materials.

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