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Concentrations of 239Pu and 240Pu in 163 surface soil samples and five soil cores collected from the northeast and north China were analyzed using the radiochemical separation combined with inductively coupled plasma mass spectrometry measurement. The average 240Pu/239Pu atomic ratios (0.185 ± 0.018) for all surface soil samples indicated that the global fallout is the major source of plutonium in the studied region. The 239,240Pu concentrations of the surface soil ranged from 0.002 mBq/g to 4.82 mBq/g, lying in the range of the reported results in the areas with similar latitude, except for a few samples. The distribution of 239,240Pu in this region is controlled by the deposition of plutonium in the atmosphere and its preservation in the soil, which were affects by multi-factors such as topography, climate, utilization of the land and vegetation coverage. The analytical results could be used as the baseline data for the assessment of the impact of nuclear activities in the past and the future. [Display omitted] • Global fallout is the major source of plutonium in the Northeast China. • The topography and precipitation are key factor for the deposition of Pu. • The westerlies and monsoon are important for Pu distribution in north China. • Land use and vegetation are important for reservation of Pu in soil. [ABSTRACT FROM AUTHOR]

Rapid bioassay method for plutonium in urine samples are employed to assess the possible internal dose resulting from exposure to plutonium in the event of a radiological and nuclear emergency. In this work, a rapid method for the determination of plutonium isotopes (239Pu and 240Pu) in large volume of urine samples was developed using tandem quadrupole ICP-MS combined with a high-efficiency sample introduction system (APEX-Ω). The mixture gases of NH 3 and He was employed to effectively eliminate the tailing of 238U and the uranium hydride ions (238U1H+and 238U1H 2 +) and significantly improve the measurement sensitivity of plutonium. The method was validated by analyzing urine samples spiked with known amounts of 239Pu and 240Pu ranging from 1 to 60 fg. The detection limits for the method were estimated to be 0.83 fg for 239Pu, 0.14 fg for 240Pu in 1 L of urine. [Display omitted] • Tandem quadrupole ICP-MS was utilized to measure Pu isotopes in large volume of urine samples. • The interference of 238U (0.23 cps) would be much less a concern at 4.0 mL min−1 NH 3 and 3.0 mL min−1 He. • The detection limits of 239Pu (0.83 fg/L) and 240Pu (0.14 fg/L) are suitable for Pu routine analysis of urine. [ABSTRACT FROM AUTHOR]

To accurately determine ultra-trace Pu isotopes in small environmental samples, we explored ICP-MS/MS in NH 3 –He mode, and investigated mechanism of 238U interference removal and measurement sensitivity improvement for plutonium isotopes. The interference of uranium and uranium hydrides was effectively eliminated using 0.4 mL/min NH 3 as reaction gas by shifting them to U(NH m) n + and UH(NH m) n +. The overall interference of uranium was reduced to <2.4 × 10−7, while remaining excellent 239Pu sensitivity (13,900 Mcps/(mg/L)) mainly due to ion focusing effect of Pu by helium gas. On this basis, the purification of plutonium using a single AG1- × 4 column was proved to be sufficient for accurate determination of plutonium isotopes by the developed detection method, and the detection limits for the method were estimated to be 0.16 fg (0.4 μBq) for 239Pu, 0.046 fg (0.4 μBq) for 240Pu and 0.039 fg (0.15 mBq) for 241Pu. The method was validated by analyzing plutonium isotopes in certificated reference materials and reported environmental samples of only 1–2 g. The analytical results of ultra-trace Pu isotopes in small amounts (∼1 g) of lake sediments obtained by the developed method were successfully applied to sediment dating. [Display omitted] • The overall interference of uranium was reduced to <2.4 × 10−7 by mass-shift mode. • Ion focusing effect of Pu by He gas and KED resulted in excellent Pu sensitivity. • Single AG1- × 4 column is sufficient for accurate measurement of Pu in small samples. • Low detection limits of 0.4 μBq for both 239Pu and 240Pu and 0.15 mBq for 241Pu. • Measured results of ultra-trace Pu isotopes succeed in sediment dating application. [ABSTRACT FROM AUTHOR]