High-precision measurement of U-Pu-Np-Am concentrations and isotope ratios in environmental reference materials by mass spectrometry

Goldstein, Steven J.; Price, Allison; Hinrichs, Kimberly A.; LaMont, Stephen P.; Nunn, A. J.; Amato, Ronald S.; Cardon, Annelise M. R.; Gurganus, Daniel W.

doi:10.1016/j.jenvrad.2021.106689

Cited by 9 publications

(6 citation statements)

References 37 publications

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“…Re-analysis of a suite of environmental CRMs, including some soils and sediments, produced towards the end of the 20 th century for the actinide elements gave 27 results that agreed with literature or certified values but had lower uncertainties. The authors recommended that many of these CRMs should be re-certified using modern high-precision MS data.…”

Section: Analysis Of Soils Plants and Related Materialssupporting

confidence: 53%

“…Provisional Hf 176 /Hf 177 , Nd 143 /Nd 144 and Sr 87 /Sr 86 data were reported. Similarly, the NIST SRM 1648a (urban particulate matter) and NIST SRM 1649a (urban dust) were analysed 27 by MC-TIMS and MC-ICP-MS to determine the Am, Np, Pu and U contents and isotopic ratios. The high Np, Pu and U concentrations measured in these two SRMs are indicative perhaps of the legacy of atmospheric fall-out of radioactive particles from nuclear bomb tests.…”

Section: Reference Materials Calibrants and Interlaboratory Comparisonsmentioning

confidence: 99%

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Atomic spectrometry update – a review of advances in environmental analysis

Bacon

Butler

Cairns

et al. 2023

J. Anal. At. Spectrom.

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Section: Analysis Of Soils Plants and Related Materialssupporting

confidence: 53%

Section: Reference Materials Calibrants and Interlaboratory Comparisonsmentioning

confidence: 99%

Atomic spectrometry update – a review of advances in environmental analysis

Bacon

Butler

Cairns

et al. 2023

J. Anal. At. Spectrom.

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“…The developed procedures for actinide extraction were verified using certified reference material available from the International Atomic Energy Agency (IAEA), i.e., Irish Sea water (IAEA-381) and sediment . Literature values for 233,236 U are not certified, neither for water nor for sediment, as well as for 237 Np in sediment, but information values (Povinec et al, 2002;Pham et al, 2008;Hain et al, 2020) or individual studies (Lee et al, 2008;Goldstein et al, 2021) are available for comparison. The new procedures were applied to ocean water samples collected at a station in the northwest Pacific Ocean (BD04, 37 • 49 N, 143 • 53 E, maximum depth 600 m) collected during the cruise KH-12-4 (GP02) of the ship R/V Hakuho Maru as part of the GEOTRACES program on August 24/25, 2012.…”

Section: Samplesmentioning

confidence: 99%

Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers

et al. 2022

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Recent major advances in Accelerator Mass Spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) regarding detection efficiency and isobar suppression have opened possibilities for the analysis of additional long-lived radionuclides at ultra-low environmental concentrations. These radionuclides, including 233U, 135Cs, 99Tc, and 90Sr, will become important for oceanographic tracer application due to their generally conservative behavior in ocean water. In particular, the isotope ratios 233U/236U and 137Cs/135Cs have proven to be powerful fingerprints for emission source identification as they are not affected by elemental fractionation. Improved detection efficiencies allowed us to analyze all major long-lived actinides, i.e., 236U, 237Np, 239,240Pu, 241Am as well as the very rare 233U, in the same 10 L water samples of a depth profile from the northwest Pacific Ocean. For this purpose, a simplified and very flexible chemical purification procedure based on extraction chromatography (a single UTEVA® column) was implemented which can be extended by a DGA® column for Am purification. The procedure was validated with the reference materials IAEA-381/385. With the additional increase in ionization efficiency expected for the extraction of actinides as fluoride molecules from the AMS ion source, a further reduction of chemical processing may become possible. This method was successfully applied to an exemplary set of air filter samples. In order to determine the quantitative 237Np concentration reliably, a 236Np spike material is being developed in collaboration with the University of Tsukuba, Japan. Ion-Laser Interaction Mass Spectrometry (ILIAMS), a novel technique for the efficient suppression of stable isobaric background, has been developed at VERA and provides unprecedented detection sensitivity for the fission fragments 135Cs, 99Tc, and 90Sr. The corresponding setup is fully operational now and the isobar suppression factors of >105 achieved, in principle, allow for the detection of the mentioned radionuclides in the environment. Especially for 90Sr analysis, this new approach has already been validated for selected reference materials (e.g., IAEA-A-12) and is ready for application in oceanographic studies. We estimate that a sample volume of only (1–3) L ocean water is sufficient for 90Sr as well as for 135Cs analysis, respectively.

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“…The complex matrix of environmental samples with the diverse and unknown existing forms of radionuclides and the trace or ultra-trace concentration level makes accurate measurement quite difficult. Researchers have tried and improved many measurement methods [ 19 , 20 , 21 , 22 , 23 ]. The purpose of this article is to review the separation methods of 90 Sr, 239 Pu, and 240 Pu that have been released in the environment, and discuss commonly used radiometric and non-radiometric measurement methods.…”

Section: Introductionmentioning

confidence: 99%

Analytical Methods for the Determination of 90Sr and 239,240Pu in Environmental Samples

Zhong

Yang

et al. 2022

Molecules

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Artificial long-lived radionuclides such as 90Sr and 239,240Pu have been long released into the environment by human nuclear activities, which have a profound impact on the ecological environment. It is of great significance to monitor the concentration of these radionuclides for environmental safety. This paper summarizes and critically discusses the separation and measurement methods for ultra-trace determination of 90Sr, 239Pu, and 240Pu in the environment. After selecting the measurement method, it is necessary to consider the decontamination of the interference from matrix elements and the key elements, and this involves the choice of the separation method. Measurement methods include both radiometric methods and non-radiometric methods. Radiometric methods, including alpha spectroscopy, liquid scintillation spectrometry, etc., are commonly used methods for measuring 239+240Pu and 90Sr. Mass spectrometry, as the representative of non-radiometric measurement methods, has been regarded as the most promising analytical method due to its high absolute sensitivity, low detection limit, and relatively short sample-analysis time. Through the comparison of various measurement methods, the future development trend of radionuclide measurement is prospected in this review. The fully automatic and rapid analysis method is a highlight. The new mass spectrometer with ultra-high sensitivity shows strong analytical capabilities for extremely low concentrations of 90Sr, 239Pu, and 240Pu, and it is expected to develop determination methods with higher sensitivity and lower detection limit.

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High-precision measurement of U-Pu-Np-Am concentrations and isotope ratios in environmental reference materials by mass spectrometry

Cited by 9 publications

References 37 publications

Atomic spectrometry update – a review of advances in environmental analysis

Atomic spectrometry update – a review of advances in environmental analysis

Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers

Analytical Methods for the Determination of 90Sr and 239,240Pu in Environmental Samples

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