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

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• 作者：Shiho Asai ; Yukiko Hanzawa ; Miki Konda ; Daisuke Suzuki ; Masaaki Magara ; Takaumi Kimura ; Ryo Ishihara ; Kyoichi Saito ; Shinsuke Yamada ; Hideyuki Hirota
• 刊名：Analytical Chemistry
• 出版年：2016
• 出版时间：March 15, 2016
• 年：2016
• 卷：88
• 期：6
• 页码：3149-3155
• 全文大小：338K
• ISSN：1520-6882

文摘

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%.