Determination of Am and Cm in spent nuclear fuels by isotope dilution inductively coupled plasma mass spectrometry and isotope dilution thermal ionization mass spectrometry after separation by high-performance liquid chromatography |
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Authors: | Frédéric Chartier Michel Aubert and Mireille Pilier |
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Institution: | (1) Commissariat à l’Energie Atomique, Saclay, DCC/DPE/SPCP/LAIE, F-91191 Gif-sur-Yvette Cedex, France, FR |
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Abstract: | Elemental and isotopic determination of americium and curium in spent nuclear fuels is necessary to validate neutronic calculation
codes and for nuclear waste disposal purposes. Prior to mass spectrometric analysis, it is mandatory to perform separations
in order to eliminate isobaric interferences between U, Pu, Am and Cm. In the spent fuels samples analyzed, a separation of
U and Pu has been first realized with an anion-exchange resin. Then a rapid Am/Cm separation has been developed by high-performance
liquid chromatography (HPLC) with an on-line detection using the Am and Cm α-emission. The influence of the different parameters
on the chromatographic separation are described and discussed. Inductively coupled plasma mass spectrometry (ICP-MS) and thermal-ionization
mass spectrometry (TIMS) have been used to measure the isotopic composition of U, Am and Cm and to determine the 241Am/238U and 244Cm/238U ratios with the double spike isotope dilution method. The measurement procedures and the accuracy and precision of the results
obtained with a quadrupole ICP-MS on different spent fuels samples are discussed and compared with those obtained by TIMS,
used as a reference technique.
Received: 30 November 1998 / Revised: 8 January 1999 / Accepted: 12 January 1999 |
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