Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

• Published in: Journal of environmental radioactivity Vol. 100; no. 8; pp. 613 - 625
• Main Authors: Godoy, Maria Luiza Duarte Pinto, Godoy, José Marcus, Roldão, Luiz Alfredo, Tauhata, Luiz
• Format: Journal Article
• Language: English
• Published: Kidlington Elsevier Ltd 01.08.2009; Elsevier
• Subjects: Applied sciences; Blanks; Energy (nuclear); Environmental Monitoring; Environmental samples; Exact sciences and technology; Extraction; Geologic Sediments - chemistry; Global environmental pollution; ICP-MS; Isotope dilution; Isotopic ratio; Mass Spectrometry - methods; Plutonium; Plutonium - analysis; Pollution; Radioactivity; Safeguards; Safety - standards; Separation; Soil - analysis; Soil Pollutants, Radioactive - analysis; Uranium; Uranium - analysis; Uranium; Environmental samples; Safeguards; Isotope dilution; ICP-MS; Plutonium; Isotopic ratio; Isotopic analysis; Radioactive pollution; Round robin test; Radioisotope; Radioprotection; Quadrupole spectrometer; Analysis method; Ultrasonic nebulization; ICP mass spectroscopy; Reference material; Environment; Measurement accuracy
• ISSN: 0265-931X; 1879-1700
• DOI: 10.1016/j.jenvrad.2009.04.012

The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for 239Pu and 1 ng 238U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, 240Pu/ 239Pu, 241Pu/ 239Pu, 234U/ 238U and 235U/ 238U atomic ratio results.