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
Format: Article
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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Summary: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.
ISSN:2218-2004