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1.
Sci Rep ; 12(1): 10068, 2022 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-35778413

RESUMO

Plutonium (Pu) has been used as a mid-twentieth century time-marker in various geological archives as a result of atmospheric nuclear tests mainly conducted in 1950s. Advancement of analytical techniques allows us to measure 239Pu and 240Pu more accurately and can thereby reconstruct the Pacific Pu signal that originated from the former Pacific Proving Grounds (PPG) in the Marshall Islands. Here, we propose a novel method that couples annual banded reef building corals and nearshore anoxic marine sediments to provide a marker to precisely determine the start of the nuclear era which is known as a part of the Anthropocene. We demonstrate the efficacy of the methods using sediment obtained from Beppu Bay, Japan, and a coral from Ishigaki Island, Japan. The sedimentary records show a clear Pu increase from 1950, peaking during the 1960s, and then showing a sharp decline during the 1970s. However, a constantly higher isotope ratio between 239Pu and 240Pu suggest an additional contribution other than global fallout via ocean currents. Furthermore, single elevations in 240Pu/239Pu provide supportive evidence of close-in-fallout similar to previous studies. Coral skeletal radiocarbon displays a clear timing with the signatures supporting the reliability of the Beppu Bay sediments as archives and demonstrates the strength of this method to capture potential Anthropocene signatures.


Assuntos
Antozoários , Plutônio , Cinza Radioativa , Poluentes Radioativos da Água , Animais , Sedimentos Geológicos , Plutônio/análise , Cinza Radioativa/análise , Reprodutibilidade dos Testes , Poluentes Radioativos da Água/análise
2.
Phys Rev Lett ; 123(7): 072701, 2019 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-31491090

RESUMO

Earth is constantly bombarded with extraterrestrial dust containing invaluable information about extraterrestrial processes, such as structure formation by stellar explosions or nucleosynthesis, which could be traced back by long-lived radionuclides. Here, we report the very first detection of a recent ^{60}Fe influx onto Earth by analyzing 500 kg of snow from Antarctica by accelerator mass spectrometry. By the measurement of the cosmogenically produced radionuclide ^{53}Mn, an atomic ratio of ^{60}Fe/^{53}Mn=0.017 was found, significantly above cosmogenic production. After elimination of possible terrestrial sources, such as global fallout, the excess of ^{60}Fe could only be attributed to interstellar ^{60}Fe which might originate from the solar neighborhood.

3.
Sci Total Environ ; 678: 603-610, 2019 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-31085490

RESUMO

The 240Pu/239Pu atom ratio is a very effective tool for the identification of the origin of plutonium (Pu) in the soil environment. We examine a dataset of 240Pu/239Pu atom ratios determined from surface and core soils at 240 sites across China. The data were compiled from 18 separate literature sources from the last 20 years. For the first time the spatial distribution (3 latitude bands and 7 natural regions) of the weighted average 240Pu/239Pu atom ratios in Chinese soils is investigated. An area to the West of Xining City, shows a weighted average 240Pu/239Pu atom ratio of 0.167 ±â€¯0.002, lower than that of average global fallout, which likely arises from the addition of local fallout radionuclides from the Chinese nuclear weapon tests at Lop Nor between 1964 and 1980. The Yumen and Jiuquan areas of Northwest China in particular show evidence of very low ratio material from the Chinese nuclear weapon tests. Excluding the impacted area around the test site the weighted average 240Pu/239Pu ratio of 0.182 ±â€¯0.002 suggests that global fallout is the main source of Pu in most Chinese soils.

4.
Anal Chem ; 91(7): 4585-4591, 2019 04 02.
Artigo em Inglês | MEDLINE | ID: mdl-30843388

RESUMO

In the frame of studies on the safe disposal of nuclear waste, there is a great interest for understanding the migration behavior of 99Tc. 99Tc originating from nuclear energy production and global fallout shows environmental levels down to 107 atoms/g of soil (∼2 fg/g). Extremely low concentrations are also expected in groundwater after diffusion of 99Tc through the bentonite constituting the technical barrier for nuclear waste disposal. The main limitation to the sensitivity of the mass spectrometric analysis of 99Tc is the background of its stable isobar 99Ru. For ultratrace analysis, the Accelerator Mass Spectrometry (AMS) setup of the Technical University of Munich using a Gas-Filled Analyzing Magnet System (GAMS) and a 14 MV Tandem accelerator is greatly effective in suppressing this interference. In the present study, the GAMS setup is used for the analysis of 99Tc in samples of the seawater reference material IAEA-443, a peat bog lake, and groundwater from an experiment of in situ diffusion through bentonite in the controlled zone of the Grimsel Test Site (GTS) within the Colloid Formation and Migration (CFM) project. With an adapted chemical preparation procedure, measurements of 99Tc concentrations at the fg/g levels with a sensitivity down to 0.5 fg are accomplished in notably small natural water samples. The access to these low concentration levels allows for the long-term monitoring of in situ tracer tests over several years and for the determination of environmental levels of 99Tc in small samples.


Assuntos
Magnetismo , Espectrometria de Massas/métodos , Tecnécio/análise , Água Subterrânea/análise , Lagos/química , Resíduos Radioativos/análise , Poluentes Radioativos da Água/análise
5.
Acta Crystallogr B ; 67(Pt 3): 218-25, 2011 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-21586829

RESUMO

A hitherto unknown phase of sodium titanate, NaTi(3)O(6)(OH)·2H(2)O, was identified as the intermediate species in the synthesis of TiO(2) nanorods. This new phase, prepared as nanorods, was investigated by electron diffraction, X-ray powder diffraction, thermogravimetric analysis and high-resolution transmission electron microscopy. The structure was determined ab initio using electron diffraction data collected by the recently developed automated diffraction tomography technique. NaTi(3)O(6)(OH)·2H(2)O crystallizes in the monoclinic space group C2/m. Corrugated layers of corner- and edge-sharing distorted TiO(6) octahedra are intercalated with Na(+) and water of crystallization. The nanorods are typically affected by pervasive defects, such as mutual layer shifts, that produce diffraction streaks along c*. In addition, edge dislocations were observed in HRTEM images.

6.
Langmuir ; 26(5): 3590-5, 2010 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-20020761

RESUMO

Reaction pathways to SnO(2) nanomaterials through the hydrolysis of hydrated tin tetrachloride precursors were investigated. The products were prepared solvothermally starting from hydrated tin tetrachloride and various (e.g., alkali) hydroxides. The influence of the precursor base on the final morphology of the nanomaterials was studied. X-ray powder diffraction (XRD) data indicated the formation of rutile-type SnO(2). Transmission electron microscopy (TEM) studies revealed different morphologies that were formed with different precursor base cations. Data from molecular dynamics (MD) simulations provide theoretical evidence that the adsorption of the cations of the precursor base to the faces of the growing SnO(2) nanocrystals is crucial for the morphology of the nanostructures.

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