Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry

This study focused on the measurement of anthropogenic radionuclides such as americium (Am) and plutonium (Pu) in environmental samples. Plutonium isotopes, particularly <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics>...

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Main Authors: Elena Moroianu, Iuliana Stanciu, Doru Pacesila, Andreea Dima, Oana Gaza, Daniel Vasile Mosu
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Language:English
Published: MDPI AG 2025-05-01
Series:Atoms
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Online Access:https://www.mdpi.com/2218-2004/13/5/45
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author Elena Moroianu
Iuliana Stanciu
Doru Pacesila
Andreea Dima
Oana Gaza
Daniel Vasile Mosu
author_facet Elena Moroianu
Iuliana Stanciu
Doru Pacesila
Andreea Dima
Oana Gaza
Daniel Vasile Mosu
author_sort Elena Moroianu
collection DOAJ
description This study focused on the measurement of anthropogenic radionuclides such as americium (Am) and plutonium (Pu) in environmental samples. Plutonium isotopes, particularly <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>239</mn></mmultiscripts></mrow></semantics></math></inline-formula>, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>240</mn></mmultiscripts></mrow></semantics></math></inline-formula>, and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>, originated from nuclear weapons testing, nuclear power plants, and accidents like Chernobyl and Fukushima Daiichi. Accurate measurement of these isotopes, considering their half-lives and trace concentrations, provides critical information about their persistence and environmental transport. Using the 1 MV Tandetron accelerator, we expanded the measurement capabilities to include <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>. Chemical separation of these isotopes was achieved through ion chromatography, employing reference isotopes <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>242</mn></mmultiscripts></mrow></semantics></math></inline-formula> and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>243</mn></mmultiscripts></mrow></semantics></math></inline-formula> for method validation. Certified reference materials, including IAEA-410 (Bikini Atoll sediment) and Sample 05, were analyzed to ensure accuracy. We validated the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>/<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>243</mn></mmultiscripts></mrow></semantics></math></inline-formula> ratio in an Am standard (IFIN-STD-Am, our laboratory produced standard for Am), achieving a measured value of 0.158 at·at<sup>−1</sup> (3%), in good agreement with the nominal value of 0.154 at·at<sup>−1</sup>. Additionally, we determined the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msup><mo>(</mo><mn>241</mn></msup><mi>Pu</mi></mrow></semantics></math></inline-formula> + <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts><mrow><mo>)</mo></mrow><msup><mo>/</mo><mn>242</mn></msup><mi>Pu</mi></mrow></semantics></math></inline-formula> ratio in the ColPuS standard to be equal to 0.029 at ·at<sup>−1</sup> (7%). These results demonstrate the potential of AMS for improved detection of actinides at low concentrations and contribute to understanding the behavior of Pu and Am isotopes.
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spelling doaj-art-c789c2a89ab142ffb4726627a6d992082025-08-20T03:14:35ZengMDPI AGAtoms2218-20042025-05-011354510.3390/atoms13050045Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass SpectrometryElena Moroianu0Iuliana Stanciu1Doru Pacesila2Andreea Dima3Oana Gaza4Daniel Vasile Mosu5Horia Hulubei National Institute for R&D in Physics and Nuclear Engineering, 077125 Magurele, RomaniaHoria Hulubei National Institute for R&D in Physics and Nuclear Engineering, 077125 Magurele, RomaniaHoria Hulubei National Institute for R&D in Physics and Nuclear Engineering, 077125 Magurele, RomaniaHoria Hulubei National Institute for R&D in Physics and Nuclear Engineering, 077125 Magurele, RomaniaHoria Hulubei National Institute for R&D in Physics and Nuclear Engineering, 077125 Magurele, RomaniaHoria Hulubei National Institute for R&D in Physics and Nuclear Engineering, 077125 Magurele, RomaniaThis study focused on the measurement of anthropogenic radionuclides such as americium (Am) and plutonium (Pu) in environmental samples. Plutonium isotopes, particularly <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>239</mn></mmultiscripts></mrow></semantics></math></inline-formula>, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>240</mn></mmultiscripts></mrow></semantics></math></inline-formula>, and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>, originated from nuclear weapons testing, nuclear power plants, and accidents like Chernobyl and Fukushima Daiichi. Accurate measurement of these isotopes, considering their half-lives and trace concentrations, provides critical information about their persistence and environmental transport. Using the 1 MV Tandetron accelerator, we expanded the measurement capabilities to include <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>. Chemical separation of these isotopes was achieved through ion chromatography, employing reference isotopes <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Pu</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>242</mn></mmultiscripts></mrow></semantics></math></inline-formula> and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>243</mn></mmultiscripts></mrow></semantics></math></inline-formula> for method validation. Certified reference materials, including IAEA-410 (Bikini Atoll sediment) and Sample 05, were analyzed to ensure accuracy. We validated the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts></mrow></semantics></math></inline-formula>/<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>243</mn></mmultiscripts></mrow></semantics></math></inline-formula> ratio in an Am standard (IFIN-STD-Am, our laboratory produced standard for Am), achieving a measured value of 0.158 at·at<sup>−1</sup> (3%), in good agreement with the nominal value of 0.154 at·at<sup>−1</sup>. Additionally, we determined the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msup><mo>(</mo><mn>241</mn></msup><mi>Pu</mi></mrow></semantics></math></inline-formula> + <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mmultiscripts><mi>Am</mi><none></none><none></none><mprescripts></mprescripts><none></none><mn>241</mn></mmultiscripts><mrow><mo>)</mo></mrow><msup><mo>/</mo><mn>242</mn></msup><mi>Pu</mi></mrow></semantics></math></inline-formula> ratio in the ColPuS standard to be equal to 0.029 at ·at<sup>−1</sup> (7%). These results demonstrate the potential of AMS for improved detection of actinides at low concentrations and contribute to understanding the behavior of Pu and Am isotopes.https://www.mdpi.com/2218-2004/13/5/45AMSactinidesradiochemistryCRMs
spellingShingle Elena Moroianu
Iuliana Stanciu
Doru Pacesila
Andreea Dima
Oana Gaza
Daniel Vasile Mosu
Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry
Atoms
AMS
actinides
radiochemistry
CRMs
title Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry
title_full Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry
title_fullStr Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry
title_full_unstemmed Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry
title_short Quantification of Plutonium and Americium in Environmental Matrices Using Accelerator Mass Spectrometry
title_sort quantification of plutonium and americium in environmental matrices using accelerator mass spectrometry
topic AMS
actinides
radiochemistry
CRMs
url https://www.mdpi.com/2218-2004/13/5/45
work_keys_str_mv AT elenamoroianu quantificationofplutoniumandamericiuminenvironmentalmatricesusingacceleratormassspectrometry
AT iulianastanciu quantificationofplutoniumandamericiuminenvironmentalmatricesusingacceleratormassspectrometry
AT dorupacesila quantificationofplutoniumandamericiuminenvironmentalmatricesusingacceleratormassspectrometry
AT andreeadima quantificationofplutoniumandamericiuminenvironmentalmatricesusingacceleratormassspectrometry
AT oanagaza quantificationofplutoniumandamericiuminenvironmentalmatricesusingacceleratormassspectrometry
AT danielvasilemosu quantificationofplutoniumandamericiuminenvironmentalmatricesusingacceleratormassspectrometry