Preparation of Microvolume Anion-Exchange Cartridge for Inductively Coupled Plasma Mass Spectrometry-Based Determination of 237Np Content in Spent Nuclear Fuel

Microvolume anion-exchange porous polymer disk-packed cartridges were prepared for Am/Np separation, which is required prior to the measurement of Neptunium-237 (237Np) with inductively coupled plasma mass spectrometry (ICPMS). Disks with a volume of 0.08 cm3 were cut out from porous sheets having a...

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Veröffentlicht in:Analytical chemistry (Washington) 2016-03, Vol.88 (6), p.3149-3155
Hauptverfasser: Asai, Shiho, Hanzawa, Yukiko, Konda, Miki, Suzuki, Daisuke, Magara, Masaaki, Kimura, Takaumi, Ishihara, Ryo, Saito, Kyoichi, Yamada, Shinsuke, Hirota, Hideyuki
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Sprache:eng ; jpn
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Zusammenfassung:Microvolume anion-exchange porous polymer disk-packed cartridges were prepared for Am/Np separation, which is required prior to the measurement of Neptunium-237 (237Np) with inductively coupled plasma mass spectrometry (ICPMS). Disks with a volume of 0.08 cm3 were cut out from porous sheets having anion-exchange-group-containing polymer chains densely attached on the pore surface. Four different amine-based groups, N,N-dimethylaminoethyl methacrylate, trimethylammonium, diethylamine, and triethylenediamine (TEDA), were selected as the anion-exchange groups to be introduced into the porous sheets. The separation performances of Am/Np were evaluated using a standard solution of 243Am, which had the same activity as its daughter nuclide 239Np in secular equilibrium. 239Np recovery of close to 100% with practically no contamination of 243Am was achieved using the TEDA-introduced disk-packed cartridge. The time to elute 239Np from the cartridge was approximately 40 s. The TEDA-introduced disk-packed cartridge was applied to the separation of Np from a spent nuclear fuel sample to confirm its separation performance. A known amount of 243Am (239Np) was added to the spent nuclear fuel sample solution to monitor the chemical yield of Np. The chemical yield of Np calculated from a measured concentration of 239Np was 90.4%. Am leakage in the Np-eluted solution was less than 1 ppt, corresponding to 0.001% of the original Am concentration in the sample. This indicates that no additional 239Np was produced by the decay of the 243Am remaining in the Np-eluted solution, thus providing a reliable chemical yield. U, which can cause a serious spectral interference involving the peak tail from the mass spectrum of 238U, was thoroughly removed with the TEDA cartridge, providing interference-free measurement of 237Np. The concentration of 237Np obtained by ICPMS was 718 ± 12 ng/mg-U, which agrees well with the theoretically calculated value. Compared with the conventional separation technique using commercially available anion-exchange resin columns, the time required to adsorb, wash, and elute Np using the TEDA- introduced disk-packed cartridge was reduced by 75%.
ISSN:0003-2700
1520-6882
DOI:10.1021/acs.analchem.5b04330