Effect of alkali metals on the accuracy of isotope ratio measurement of uranium by ICP-MS

Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

“…However, in order to effectively achieve an accreditation, the same should be demonstrated with respect to total uranium content and isotopic composition determination. Quadrupole ICP-MS has been successfully used to determine both uranium content and isotopic ratios in environmental samples; notwithstanding, in order to obtain high precision 234 U/ 238 U and 236 U/ 238 U atomic ratio measurements, a careful chemical separation and optimization of ICP-MS operational conditions are needed Ghersini, 1975;Halicz et al, 2006;Horwitz et al, 1992;Ketterer et al, 2000;Kraemer et al, 2002;Magara et al, 2002;Policke et al, 1998;Tagami and Uchida, 2007;Uchida et al, 2000;Vanhaecke et al, 2007;Zheng et al, 2004;Zheng and Yamada, 2006).…”

“…IAEA safeguard network laboratory requirements and statements related to both uranium and plutonium total content and isotopic composition determinations are (IAEA, 2005): 1) 10% accuracy for total plutonium content and 240 Pu/ 239 Pu ratio at 0.1 ng of Pu level; 2) 10% accuracy for total uranium content and 234 U/ 238 U and 236 U/ 238 U ratios, and a 1% accuracy for 235 U/ 238 U at 10 ng of U level; 3) Be able to determine 240 Pu/ 239 Pu ratio between 0.001 and 1; 4) Be able to determine 235 U/ 238 U ratio between 0.001 and 17, 234 U/238U ratio between 0.00002 and 0.01, and 236 U/ 238 U ratio between 0.00001 and 0.01; 5) Reach a blank level of Pu 10 fg/swipe; 6) Reach a blank level of U between 0.1 and 5 ng/swipe; Several publications in the literature deal with either the determination of the plutonium isotope ratio and isotope concentration by ICP-MS (see, for example, the review published by Kim et al, 2007) or with the determination of the total uranium concentration or isotope ratio Ghersini, 1975;Halicz et al, 2006;Horwitz et al, 1992;Ketterer et al, 2000;Kraemer et al, 2002;Magara et al, 2002;Policke et al, 1998;Tagami and Uchida, 2007;Uchida et al, 2000;Vanhaecke et al, 2007;Zheng and Yamada, 2006). But there are relatively few publications related to the simultaneous determination of both uranium and plutonium isotope ratios and isotope concentrations determination by ICP-MS, much less starting from a single environmental sample aliquot Truscott et al, 2001).…”

Automatic sequential separation with an anion-exchange column for ultra-trace analysis of Pu, U, Th, Pb, and lanthanides in environmental samples

“…Cutting edge technologies in the mass spectrometry, such as laser ablation techniques [6], and inductively coupled plasma mass spectrometry (ICP-MS) with a tandem quadrupole mass separation mechanism [7] can be used to achieve trace elemental analysis of environmental samples without chemical treatment. Chemical separation is, however, still required for an accurate and precise isotopic analysis to prevent the interferences including matrix effects [8].…”

QA/QC Activities and Estimation of Uncertainty for Ultra-trace Analysis of Uranium and Plutonium in Safeguards Environmental Samples

“…[8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27] The methods and procedures were validated, for example, by the use of reference materials certified by NBL (New Brunswick Laboratory) such as CRM111A ( 233 U 29 for validation of the developed bulk and particle analytical methods. The JAEA's measurement results and capabilities were proved to be excellent in the comparisons.…”

“…In bulk analysis, the interferance of alkali metals as well as polyatomic ions, such as IrAr, PtAr, AuAr, PbO 2 , ReO 3 , WO 3 , etc., on the isotope ratio measurements of U and Pu have been well examined, and chemical separation was ≤5 % (at 1 pg SRM947) a: Corresponding to confidence level ≈ 95%, b: typical accuracy expected by IAEA; ≤20 % for 10 ng of U, c: ≤10 % for 5 pg of Pu, d: ≤1 % for 10 ng of U, e: ≤10 % for 5 pg of Pu, f: ≤10 % for 1 µm particle of UO 2 (~5 pg of U ), g: ≤1 % for 1 µm particle of UO 2 . 9,10 On the other hand, it is difficult to complement the isotope ratio measurements in the particle analysis, because it is performed without chemical separation in principle. In future, besides the UH evaluation, interference of polyatomic ions with the minor isotope ratios should be investigated.…”