Elemental and isotopic analysis of americium in non-separated spent fuels using high resolution ICP-OES and sector field ICP-MS

Abstract

As there are no matrix-matched certified reference materials, accurate and straightforward analytical procedures for the determination of americium (Am) in non-separated spent fuels employing high resolution ICP-OES and sector field (SF-) ICP-MS were developed and cross-validated. One spent (Th,Pu)O 2 fuel and two U/Pu-based spent fuels representing different chemical and isotopic compositions were analysed for their Am content. Even though the lowest limit of detection (0.07 mg kg À1) was obtained at l ¼ 283.226 nm, the ICP-OES signal at l ¼ 408.929 nm provided the most accurate results for the analysis of the spent fuel among the six investigated Am emission wavelengths. Massive spectral interference from Th precluded the use of the l ¼ 283.226 nm emission line for Am analysis of the (Th,Pu)O 2 fuel, while other potential interferences from plutonium (Pu) and neptunium (Np) could be excluded for all the tested Am wavelengths. Employing ICP-OES, both external calibration and standard addition yielded comparable Am amount concentrations. Calibration of the SF-ICP-MS response for Am was accomplished using both 232 Th and 238 U signals as well as applying the related mass bias. This calibration methodology that is frequently used in the absence of an Am stock standard solution was tested against a home-made 241 Am stock standard solution underlining the validity of this calibration approach. Sector field ICP-MS analysis essentially confirmed the Am concentrations obtained using ICP-OES in the three spent fuel solutions with mean values overlapping within their standard deviations. Considering isotopes of other actinides such as Pu and curium (Cm), the Am isotopic abundance (241 Am, 242 Am, 243 Am) was established in two non-separated fuel solutions comparing well with model calculations based on the ORIGEN-2 code.

A review on the mass spectrometric studies of americium: Present status and future perspective

“…ICPMS is a popular mass spectrometric technique to determine concentrations and isotope ratios of Am and other actinide elements (Agarande et al, ; Truscott et al, ; Boulyga et al, ; Lee et al, ; Hang et al, ; Pointurier, Baglan, & Hemet, ; Wang, Chen, & Chiu, ; Epov et al, ; Lee et al, ; Varga, ; Varga et al, ,; Zheng & Yamada, ; Guerin et al, ; Krachler et al, ). In ICP, the M + ions are produced with generation of plasma (with Ar gas) at atmospheric pressure, and introduction of the sample into the spray chamber with a pneumatic nebulizer.…”

“…Determination of isotopic composition of Am and concentration in irradiated nuclear fuels is required in nuclear technology for various reasons. For example, the experimental data on the isotopic composition and concentration of Am are important to develop and validate theoretically predictive ORIGEN (Oak Ridge Isotope Generation) code and neutronic code (Krachler et al, ). Additionally, experiments are underway to study the feasibility to burn plutonium in existing light‐water reactors, and to reduce the production of other minor actinides (Am, Np, Cm).…”

“…Additionally, experiments are underway to study the feasibility to burn plutonium in existing light‐water reactors, and to reduce the production of other minor actinides (Am, Np, Cm). The determination of Am concentration is important to study the effectiveness of burning minor‐actinides with test fuel samples (Guerin et al, ; Krachler et al, ).…”

“…At JRC‐ITU, Karlsruhe, Germany (Krachler et al, ), the dissolved solutions from two spent fuels MET 1–4 and 1–7 were used to determine the isotopic composition and concentration of Am with sector‐field ICPMS. Because no reference material of Am is available commercially to check the validity of the methodology, ICP‐OES based on an independent physico‐chemical principle was also employed to compare the results of Am concentration (Krachler et al, ). The fuel samples were dissolved in a hot‐cell at JRC‐ITU in a mixture of 3 M HNO 3 and 0.2 M HF, and the solutions were diluted with 1 M HNO 3 (dilution factor of 9,000) for analysis with ICPMS.…”

Polymer based sorbent materials for thermal ionization mass spectrometric determination of uranium(vi) and plutonium(iv) ions

“…[1][2][3][4][5][6][7] However, TIMS involves a multistep sample manipulation to eliminate the undesirable matrix and loading of a small volume of solution on a lament for thermal ionization. [9][10][11][12] Zheng et al have reviewed different atomic spectrometric techniques, including TIMS and ICP-MS, being used for the objective of radiation protection, and observed that TIMS has been gradually replaced by MC-ICP-MS in the elds of nuclear chemistry and geochemistry. [9][10][11][12] Zheng et al have reviewed different atomic spectrometric techniques, including TIMS and ICP-MS, being used for the objective of radiation protection, and observed that TIMS has been gradually replaced by MC-ICP-MS in the elds of nuclear chemistry and geochemistry.…”