More than Five Percent Ionization Efficiency by Cavity Source Thermal Ionization Mass Spectrometry for Uranium Subnanogram Amounts

Type Article
Date 2019-05
Language English
Author(s) Trinquier AnneORCID1, Maden Colin1, Faure Anne-Laure2, Hubert Amélie2, Pointurier Fabien2, Bourdon Bernard3, Schönbächler Maria1
Affiliation(s) 1 : ETH Zürich, Institute of Geochemistry and Petrology, Clausiusstrasse 25, CH-8092 Zürich, Switzerland
2 : CEA, DAM, DIF, 91297 Arpajon Cedex, France
3 : Laboratoire de Géologie de Lyon, ENS Lyon and UCBL, UMR 5276, CNRS, France
Source Analytical Chemistry (0003-2700) (American Chemical Society (ACS)), 2019-05 , Vol. 91 , N. 9 , P. 6190-6199
DOI 10.1021/acs.analchem.9b00849
WOS© Times Cited 5
Abstract

Numerous applications require the precise analysis of U isotope relative enrichment in sample amounts in the sub-nanogram to picogram range, among those are nuclear forensics, nuclear safeguards, environmental survey and geosciences. However, conven-tional thermal ionization mass spectrometry (TIMS) yields U combined ionization and transmission efficiencies (i.e ratio of ions detected to sample atoms loaded) less than 0.1 or 2% depending on the loading protocol, motivating the development of sources capable of enhancing ionization. The new prototype cavity source TIMS at ETH offers improvements from 4 to 15 times in com-bined ionization and transmission efficiency compared to conventional TIMS, yielding up to 5.6 % combined efficiency. Uranium isotope ratios have been determined on reference standards in the 100 pg range bound to ion-exchange or extraction resin beads. For natural U standards, n(235U)/n(238U) ratios are measured to relative external precisions of 0.5 to 1.0 % (2RSD, 2<n<11, conven-tional source) or 2.0 % (2RSD, n=6, cavity source) and accuracies of 0.2 to 0.7 % (conventional source) or 0.4-0.9 % (cavity source). Meanwhile, n(234U)/n(238U) ratios are determined to relative external precisions of 1.7 to 3.6 % (2RSD, 2<n<11, conven-tional source) or 5.6 % (2RSD, n=6, cavity source) and accuracies of 0.1 to 2.5% (conventional source) or 0.5 to 8.3% (cavity source), which would benefit further from in-run organic interference and peak tailing corrections.

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Trinquier Anne, Maden Colin, Faure Anne-Laure, Hubert Amélie, Pointurier Fabien, Bourdon Bernard, Schönbächler Maria (2019). More than Five Percent Ionization Efficiency by Cavity Source Thermal Ionization Mass Spectrometry for Uranium Subnanogram Amounts. Analytical Chemistry, 91(9), 6190-6199. Publisher's official version : https://doi.org/10.1021/acs.analchem.9b00849 , Open Access version : https://archimer.ifremer.fr/doc/00489/60037/