Simultaneous Determination of Transuranium Radionuclides for Nuclear Forensics by Compact Accelerator Mass Spectrometry

Anal Chem. 2023 Feb 21;95(7):3647-3655. doi: 10.1021/acs.analchem.2c04544. Epub 2023 Feb 10.

Abstract

Accelerator mass spectrometry (AMS) is one of the most sensitive techniques used to measure the long-lived actinides. This is particularly of interest for determination of ultra-trace transuranium nuclides and their isotopic fingerprints for nuclear forensics. In this work, a new method was developed for simultaneous determination of transuranium nuclides (Np, Pu, Am, and Cm isotopes) by using 300 kV AMS after a sequential chemical separation of each group of actinides. 242Pu and 243Am were utilized as tracers for Np/Pu and Am/Cm yield monitoring. The results show that the chemical behaviors of Np and Pu on the TK200 column and those of Am and Cm on the DGA column were very consistent in 8-9 mol/L of HNO3 and 0.015-0.03 mol/L of NaNO2 media during the radiochemical separation. The AMS detection efficiencies for transuranium nuclides were also evaluated. The detection limits for all radionuclides are below femtogram level and even in attogram level for Pu and Cm isotopes. The established method has been successfully applied to accurately measure various transuranium nuclides in a single actinide radionuclide solution, demonstrating its feasibility for nuclear forensic investigation.