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Etude des réactions "ions - molécules" en phase gazeuse dans les dispositifs de collision réaction : Application à la résolution directe des interférences spectroscopiques en ICP-MS.

Georges Favre 1
1 LANIE - Laboratoire de développement Analytique Nucléaire Isotopique et Elémentaire
SEARS - Service d'études analytiques et de réactivité des surfaces : DEN/DPC
Abstract : Inductively Coupled Plasma Mass Spectrometry emerged as the most widespread mass spectrometry technique in inorganic analytical chemistry for determining the concentration of a given isotope or measuring isotope ratio, because of its numerous assets, which in particular its sensitivity and its short analysis time. The problem of spectroscopic interferences, inherent to this technique, finds a solution through the use of collision-reaction devices. An in situ interference removal is feasible with the addition of a well selected gas in the collision-reaction cell. The chemical separation steps, commonly used before the measure and very restrictive on radioactive samples, can be avoided by this way. The understanding of the chemistry of "ions-molecules" interactions in the gas phase is however fundamental to optimize the efficiency of such devices. Thus, an accurate knowledge of experimental conditions in the reaction zone appears crucial in order to interpret observed reactivities.

Two ICP-MS with different design, the X7 Quadrupole ICP-MS (Thermo-Fisher Scientific) and the Isoprobe Multi-Collection ICP-MS (GV Instruments), have been used in this work. The experimental conditions in the collision-reaction cell of each instrument are determined according to instrumental parameters. This preliminary study is then used for the resolution of two nuclear field characteristic interferences. A theoretical approach by using quantum chemistry calculations enables to interpret the formation of zirconium oxides, responsible for the removal of 90Zr+ interferent ion, when O2 is used in the cell to measure the 90Sr radionuclide. The reactivity of five lanthanide cations (Nd, Sm, Eu, Gd and Dy) with several gases (O2, N2O, CO2, NH3) is also experimentally studied. The effectiveness of ammonia for solving Eu/Gd isobaric interferences is underlined. A periodicity in reactivity above the lanthanides series, due to the electronic configuration of Ln+ cations ground state, is proposed to explain the observed differences of behaviour.
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Georges Favre. Etude des réactions "ions - molécules" en phase gazeuse dans les dispositifs de collision réaction : Application à la résolution directe des interférences spectroscopiques en ICP-MS.. Autre. Université d'Evry-Val d'Essonne, 2008. Français. ⟨tel-00348445⟩

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