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Determination of Femtogram-Level Plutonium Isotopes in Environmental and Forensic Samples with High-Level Uranium Using Chemical Separation and ICP-MS/MS Measurement
journal contribution
posted on 2019-08-23, 19:33 authored by Xiaolin Hou, Weichao Zhang, Yanyun WangICP-MS is becoming
a competitive technique for measurement of plutonium
isotopes. Besides the abundance sensitivity (tailing of 238U to m/z = 239 and 240), isobaric
and polyatomic ions interferences (e.g., 238U1H+) are the most critical challenges for determination
of low-level plutonium in high uranium samples. This work presents
a new method to solve this problem using ICP-MS with two tandem quadrupole
separators and a dynamic collision/reaction cell combined with chemical
separation. The interference of uranium hydrides (238U1H+ and 238U1H2+) was effectively eliminated using CO2 as
reaction gas by converting hydrides to oxides of uranium ions (UO+/UO2+) but still keeping the intensity
of the Pu+ signal. The tailing interference of 238U+ (abundance sensitivity) was intensively eliminated
by significantly suppressing the 238U+ signal
using CO2 as reaction gas and using two tandem quadrupole
mass separators in the ICP-MS/MS. With these approaches the overall
interference of uranium was reduced to <1 × 10–8, which is 3 orders of magnitude better than the conventional ICP-MS.
Combined with chemical separation with a decontamination factor of
105 for uranium, an overall factor of 1012 for
elimination of uranium interference was achieved. The developed method
was demonstrated to enable accurate determination of <10–15 g/g level plutonium isotopes in environmental samples even in a
uranium debris sample with a U/Pu atomic ratio of up to 1012. The developed method was validated by analysis of a spiked solution
and certified reference materials of soil.