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Comparison of thermal ionization mass spectrometry and Multiple Collector Inductively Coupled Plasma Mass Spectrometry for cesium isotope ratio measurements

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Title: Comparison of thermal ionization mass spectrometry and Multiple Collector Inductively Coupled Plasma Mass Spectrometry for cesium isotope ratio measurements
Authors: Isnard, H.1 helene.isnard@cea.fr, Granet, M.1, Caussignac, C.1, Ducarme, E.1, Nonell, A.1, Tran, B.1, Chartier, F.2
Source: Spectrochimica Acta Part B. Nov2009, Vol. 64 Issue 11/12, p1280-1286. 7p.
Subjects: Comparative studies, Mass spectrometry, Inductively coupled plasma mass spectrometry, Cesium isotopes, Nuclear fuels, Separation (Technology)
Abstract: Abstract: In the nuclear domain, precise and accurate isotopic composition determination of elements in spent nuclear fuels is mandatory to validate neutron calculation codes and for nuclear waste disposal. The present study presents the results obtained on Cs isotope ratio by mass spectrometric measurements. Natural cesium is monoisotopic (133Cs) whereas cesium in spent fuels has 4 isotopes (133Cs, 134Cs, 135Cs, and 137Cs). As no standard reference material is available to evaluate the accuracy of Cs isotopic measurements, a comparison of cesium isotopic composition in spent nuclear fuels has been performed between Thermal Ionization Mass Spectrometry (TIMS) and a new method involving Multiple Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICPMS) measurements. For TIMS measurements, isotopic fractionation has been evaluated by studying the behavior of cesium isotope ratios (133Cs/137Cs and 135Cs/137Cs) during the analyses. For MC-ICPMS measurements, the mass bias effects have been corrected with an external mass bias correction using elements (Eu and Sb) close to cesium masses. The results obtained by the two techniques show good agreement: relative difference on 133Cs/137Cs and 135Cs/137Cs ratios for two nuclear samples, analyzed after chemical separation, ranges from 0.2% to 0.5% depending on the choice of reference value for mass bias correction by MC-ICPMS. Finally the quantification of the 135Cs/238U ratio by the isotope dilution technique is presented in the case of a MOx (mixed oxide) spent fuel sample. Evaluation of the global uncertainties shows that this ratio could be defined at an uncertainty of 0.5% (k =2). The intercomparison between two independent mass spectrometric techniques is fundamental for the evaluation of uncertainty when no isotopic standard is available. [Copyright &y& Elsevier]
Copyright of Spectrochimica Acta Part B is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Comparison of thermal ionization mass spectrometry and Multiple Collector Inductively Coupled Plasma Mass Spectrometry for cesium isotope ratio measurements
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  Data: <searchLink fieldCode="AR" term="%22Isnard%2C+H%2E%22">Isnard, H.</searchLink><relatesTo>1</relatesTo><i> helene.isnard@cea.fr</i><br /><searchLink fieldCode="AR" term="%22Granet%2C+M%2E%22">Granet, M.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Caussignac%2C+C%2E%22">Caussignac, C.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Ducarme%2C+E%2E%22">Ducarme, E.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Nonell%2C+A%2E%22">Nonell, A.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Tran%2C+B%2E%22">Tran, B.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Chartier%2C+F%2E%22">Chartier, F.</searchLink><relatesTo>2</relatesTo>
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  Data: <searchLink fieldCode="JN" term="%22Spectrochimica+Acta+Part+B%22">Spectrochimica Acta Part B</searchLink>. Nov2009, Vol. 64 Issue 11/12, p1280-1286. 7p.
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  Data: <searchLink fieldCode="DE" term="%22Comparative+studies%22">Comparative studies</searchLink><br /><searchLink fieldCode="DE" term="%22Mass+spectrometry%22">Mass spectrometry</searchLink><br /><searchLink fieldCode="DE" term="%22Inductively+coupled+plasma+mass+spectrometry%22">Inductively coupled plasma mass spectrometry</searchLink><br /><searchLink fieldCode="DE" term="%22Cesium+isotopes%22">Cesium isotopes</searchLink><br /><searchLink fieldCode="DE" term="%22Nuclear+fuels%22">Nuclear fuels</searchLink><br /><searchLink fieldCode="DE" term="%22Separation+%28Technology%29%22">Separation (Technology)</searchLink>
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  Data: Abstract: In the nuclear domain, precise and accurate isotopic composition determination of elements in spent nuclear fuels is mandatory to validate neutron calculation codes and for nuclear waste disposal. The present study presents the results obtained on Cs isotope ratio by mass spectrometric measurements. Natural cesium is monoisotopic (133Cs) whereas cesium in spent fuels has 4 isotopes (133Cs, 134Cs, 135Cs, and 137Cs). As no standard reference material is available to evaluate the accuracy of Cs isotopic measurements, a comparison of cesium isotopic composition in spent nuclear fuels has been performed between Thermal Ionization Mass Spectrometry (TIMS) and a new method involving Multiple Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICPMS) measurements. For TIMS measurements, isotopic fractionation has been evaluated by studying the behavior of cesium isotope ratios (133Cs/137Cs and 135Cs/137Cs) during the analyses. For MC-ICPMS measurements, the mass bias effects have been corrected with an external mass bias correction using elements (Eu and Sb) close to cesium masses. The results obtained by the two techniques show good agreement: relative difference on 133Cs/137Cs and 135Cs/137Cs ratios for two nuclear samples, analyzed after chemical separation, ranges from 0.2% to 0.5% depending on the choice of reference value for mass bias correction by MC-ICPMS. Finally the quantification of the 135Cs/238U ratio by the isotope dilution technique is presented in the case of a MOx (mixed oxide) spent fuel sample. Evaluation of the global uncertainties shows that this ratio could be defined at an uncertainty of 0.5% (k =2). The intercomparison between two independent mass spectrometric techniques is fundamental for the evaluation of uncertainty when no isotopic standard is available. [Copyright &y& Elsevier]
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  Data: <i>Copyright of Spectrochimica Acta Part B is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1016/j.sab.2009.10.004
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      – SubjectFull: Inductively coupled plasma mass spectrometry
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      – SubjectFull: Cesium isotopes
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      – SubjectFull: Separation (Technology)
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      – TitleFull: Comparison of thermal ionization mass spectrometry and Multiple Collector Inductively Coupled Plasma Mass Spectrometry for cesium isotope ratio measurements
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              Text: Nov2009
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