<Superscript>239, 240, 241</Superscript>Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

Sector field inductively coupled plasma mass spectrometry (SF-ICPMS) has been used with analysis of solution samples and laser ablation (LA) of electrodeposited alpha sources to characterize plutonium activities and atom ratios prevalent in the western USA. A large set of surface soils and attic dusts were previously collected from many locations in the states of Nevada, Utah, Arizona, and Colorado; specific samples were analyzed herein to characterize the relative contributions of stratospheric fallout vs. Nevada Test Site (NTS) plutonium. This study illustrates two different ICPMS-based analytical strategies that are successful in fingerprinting Pu in environmental soils and dusts. Two specific datasets have been generated: (1) soils are leached with HNO₃-HCl, converted into electrodeposited alpha sources, counted by alpha spectrometry, then re-analyzed using laser ablation SF-ICPMS; (2) samples are completely dissolved by treatment with HNO₃-HF-H₃BO₃, Pu fractions are prepared by extraction chromatography, and analyzed by SF-ICPMS. Optimal laser ablation and ICPMS conditions were determined for the re-analysis of archived alpha spectrometry “planchette” sources. The best ablation results were obtained using a large spot size (200 μm), a defocused beam, full repetition rate (20 Hz) and scan rate (200 μm s⁻¹); LA-ICPMS data were collected with a rapid electrostatic sector scanning experiment. Less than 10% of the electroplated surface area is consumed in the LA-ICPMS analysis, which would allow for multiple re-analyses. Excellent agreement was found between ^239+240Pu activities determined by LA-ICPMS vs. activity results obtained by alpha spectrometry for the same samples ten years earlier. LA-ICPMS atom ratios for ²⁴⁰Pu/²³⁹Pu and ²⁴¹Pu/²³⁹Pu range from 0.038–0.132 and 0.00034–0.00168, respectively, and plot along a two-component mixing line (²⁴¹Pu/²³⁹Pu = 0.013 [²⁴⁰Pu/²³⁹Pu] – 0.0001; r ² = 0.971) with NTS and global fallout end-members. A rapid total dissolution procedure, followed by extraction chromatography and SF-ICPMS solution Pu analysis, generates excellent agreement with certified ^239+240Pu activities for standard reference materials NIST 4350b, NIST 4353, NIST 4357, and IAEA 385. ^239+240Pu activities and atom ratios determined by total dissolution reveal isotopic information in agreement with the LA-ICPMS dataset regarding the ubiquitous mixing of NTS and stratospheric fallout Pu sources in the regional environment. For several specific samples, the total dissolution method reveals that Pu is incompletely recovered by simpler HNO₃-HCl leaching procedures, since some of the Pu originating from the NTS is contained in refractory siliceous particles.     

Monte Carlo modelling of human body for dose conversion coefficients of 137Cs in soil of the Eastern Black Sea region of Turkey

Absorbed dose conversion coefficients for a human body standing on the soil surface were calculated for ¹³⁷Cs in the soil of Eastern Black Sea region of Turkey using the Monte Carlo simulation method. The results were given in nGy h^?1 per Bq cm^?2 as a function of depth. Simple numerical integration of this function multiplied with the known specific activity as a function of depth gives the absorbed dose conversion coefficients for any distribution of ¹³⁷Cs in soil. Gaussian distribution of ¹³⁷Cs in the soil was considered for calculations.     

Determination of isotopic composition of plutonium in hot particles of the Chernobyl area

The knowledge of the isotopic composition of man-made transuranium elements (TUE) in the environmental samples is of great interest because, on the basis of these data, statements about the origin of the TUE can be made. One of the most radiotoxic elements released during reactor accidents and nuclear weapons tests was plutonium with the alpha emitters ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu, ²⁴²Pu and the beta-emitter ²⁴¹Pu which decays into ²⁴¹Am. The determination of plutonium in “hot” particles from the Chernobyl reactor was accomplished by means of solid state nuclear track detectors registering the alpha particles and by alpha spectroscopy after chemical treatment. Furthermore, in order to perform a complete analysis of the isotopic composition one of the “hot” particles has been investigated by resonance ionization mass spectrometry which possesses an excellent sensitivity and a good isotopic resolution.     

Potre-H: A Dynamic Model for Rationuclide Transport in Agricultural Ecosystems

Abstract

This paper presents a dynamic compartment model that simulates the transfer of radionuclides through components of agricultural systems following deposition to ground, and predicts the resulting concentrations in food products. The system of linear differential equations corresponding to this model was solved analytically for release in the dormant season, before or after sowing, and for release in the growing season as a single or time dependent deposition. Model predictions have also been compared with levels ¹³¹I and ¹³⁷Cs in grass and milk resulting from the Chernobyl accident.     

氢化物-原子荧光光谱法测定大气沉降物中砷含量

大气沉降物中砷的测定传统方法干扰多,本文针对大气沉降物样品的复杂性,在样品中加入盐酸、硝酸、高氯酸于电热板上加热消解,能有效的消除大量有机质对测量结果的干扰,为大气沉降物研究工作提供更为精准的检测数据。该方法能有效的消除基体干扰,分析成本低,测定的精密度高、准确性好,相对标准偏差(RSD)低于2.0%,样品加标回收率高于90%。     

Probleme,Methoden, Analysen- und Meßverfahren im nuklearen Umweltschutz

Es werden die wesentlichsten Probleme und Aufgaben des Umweltschutzes hinsichtlich der verschiedenen Komponenten der natürlichen und zivilisatorischen Strahlenbelastung, die Überwachung auf Radioaktivität als Folge der Kernwaffenversuche und die Umgebungsüberwachung von Kernanlagen beschrieben.

Es wird ein Überblick über die verschiedenen Bestimmungsmethoden der Radionuklide, die Schritte der Probenaufbereitung, die zur Alpha-, Beta- und Gammamessung verwendeten Verfahren sowie die Meßwertverarbeitung gegeben.     

Eine Methode der 90Sr-45Ca-Simultanbestimmung

Von den radioaktiven Falloutprodukten ist das ⁹⁰Sr bei weitem das gefährlichste, da es von den Pflanzen und Tieren wegen seiner chemischen Verwandtschaft zum Calcium wie dieses im Organismus eingebaut wird und auf dem Wege der Verteilerkette Boden–Pflanze–Tier–Mensch schließlich auch im menschlichen Organismus eingebaut wird.     

Plutonium fractionation in southern Baltic Sea sediments

In this study, different chemical plutonium fractions (dissolved in water, connected to carbonates, connected to oxides, complexed with organic matter, mineral acids soluble and the rest) in sediments from the Vistula River estuary, the Gdańsk Basin and the Bornholm Deep were determined. The distribution of ^239+240Pu in analysed sediments samples was not uniform but dependent on its chemical form, depth and the sediment geomorphology. The highest amount of plutonium exists in middle parts of sediments and comes from the global atmospheric fallout from nuclear tests in 1958–1961. According to all analysed fractions, the biggest amount of ^239+240Pu was in the mobile form, connected to carbonate fractions from the Vistula River estuary, the Gulf of Gdańsk and the Bornholm Deep sediments.     

Fission products from the damaged Fukushima reactor observed in Hungary

Fission products, especially ¹³¹I, ¹³⁴Cs and ¹³⁷Cs, from the damaged Fukushima Dai-ichi nuclear power plant (NPP) were detected in many places worldwide shortly after the accident caused by natural disaster. To observe the spatial and temporal variation of these isotopes in Hungary, aerosol samples were collected at five locations from late March to early May 2011: Institute of Nuclear Research, Hungarian Academy of Sciences (ATOMKI, Debrecen, East Hungary), Paks NPP (Paks, South-Central Hungary) as well as at the vicinity of Aggtelek (Northeast Hungary), Tapolca (West Hungary) and Bátaapáti (Southwest Hungary) settlements. In addition to the aerosol samples, dry/wet fallout samples were collected at ATOMKI, and airborne elemental iodine and organic iodide samples were collected at Paks NPP. The peak in the activity concentration of airborne ¹³¹I was observed around 30 March (1–3 mBq m^?3 both in aerosol samples and gaseous iodine traps) with a slow decline afterwards. Aerosol samples of several hundred cubic metres of air showed ¹³⁴Cs and ¹³⁷Cs in detectable amounts along with ¹³¹I. The decay-corrected inventory of ¹³¹I fallout at ATOMKI was 2.1±0.1 Bq m^?2 at maximum in the observation period. Dose-rate contribution calculations show that the radiological impact of this event at Hungarian locations was of no considerable concern.