In this study, the Pb/U fractionation between zircon and uraninite during femtosecond Laser Ablation Inductively Coupled Plasma Mass Spectrometry （fs-LA-ICP-MS） analysis was studied in detail. The results show signi...In this study, the Pb/U fractionation between zircon and uraninite during femtosecond Laser Ablation Inductively Coupled Plasma Mass Spectrometry （fs-LA-ICP-MS） analysis was studied in detail. The results show significant Pb/U fractionation between zircon and uraninite during fs-LA-ICP-MS analysis that when calibrated against the zircon standard M257, the obtained U-Pb age of the Chinese national uraninite standard GBW04420 is 17% older than the recommended value. Thus, the accurate in-situ U-Pb dating of uraninite by LA-ICP-MS requires matrix-matched external standards for calibration. Uraninite in thin sections of two U-mineralized leucogranite from the Gaudeanmus in Namibia was analyzed by a fs-LA-ICP-MS equipped with a Signal Smooth Device （SSD）, using laser spot and frequency of 10 μm and 1 Hz, respectively. When calibrated using GBW04420 as the external standard, two samples give weighted mean 2066pb/238U ages of 504±3 Ma （2σ, n=21） and 503±3 Ma （2σ, n=22）, and only one of two samples yields a concordia U-Pb age of 507±1 Ma （2or, n=21）. These results are consistent with ID-TIMS U-Pb ages of 509±1 and 508±12 Ma and are also indistinguishable from zircon U-Pb upper intercept ages of 506±33 Ma （2σ, n=29） and 501±51 Ma （2σ, n=29）. The present study shows that in-situ U-Pb dating of uraninite can deliver more reliable formation ages of the deposit than dating coeval high-U zircon because the latter commonly suffer significant Pb loss after formation. Our results confirm that GBW04420 is an ideal matrix matching standard for in-situ U-Pb dating of uraninite.展开更多
The unique physical and chemical properties of room-temperature ionic liquids(RTILs) have recently received increasing attention as solvent alternatives for possible application in the field of nuclear industry, parti...The unique physical and chemical properties of room-temperature ionic liquids(RTILs) have recently received increasing attention as solvent alternatives for possible application in the field of nuclear industry, particularly in liquid-liquid separations of radioactive nuclides. We investigated solvent extraction of U(VI) from aqueous solutions into a commonly used ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([C4mim][NTf2]) using trioctylphosphine oxide(TOPO) as an extractant. The effects of contact time, TOPO concentration, acidity, and nitrate ions on the U(VI) extraction are discussed in detail. The extraction mechanism was proposed based on slope analysis and UV-Vis measurement. The results clearly show that TOPO/[C4mim][NTf2] provides a highly efficient extraction of U(VI) from aqueous solution under near-neutral conditions. When the TOPO concentration was 10 mmol/L, the extraction of 1 mmol/L U(VI) was almost complete(> 97%). Both the extraction efficiency and distribution coefficient were much larger than in conventional organic solvents such as dichloromethane. Slope analysis confirmed that three TOPO molecules in [C4mim][NTf2] bound with one U(VI) ion and one nitrate ion was also involved in the complexation and formed the final extracted species of [UO2(NO3)(TOPO)3]+. Such a complex suggests that extraction occurs by a cation-exchange mode, which was subsequently evidenced by the fact that the concentration of C4mim+ in the aqueous phase increased linearly with the extraction percent of U(VI) recorded by UV-Vis measurement.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.41203027 and 41473031)the State Administration of Foreign Expert Affairs of China(Grant No.B07039)the Special Fund for Basic Scientific Research of Central Colleges,China University of Geosciences(Wuhan)(Grant No.CUGL140403)
文摘In this study, the Pb/U fractionation between zircon and uraninite during femtosecond Laser Ablation Inductively Coupled Plasma Mass Spectrometry （fs-LA-ICP-MS） analysis was studied in detail. The results show significant Pb/U fractionation between zircon and uraninite during fs-LA-ICP-MS analysis that when calibrated against the zircon standard M257, the obtained U-Pb age of the Chinese national uraninite standard GBW04420 is 17% older than the recommended value. Thus, the accurate in-situ U-Pb dating of uraninite by LA-ICP-MS requires matrix-matched external standards for calibration. Uraninite in thin sections of two U-mineralized leucogranite from the Gaudeanmus in Namibia was analyzed by a fs-LA-ICP-MS equipped with a Signal Smooth Device （SSD）, using laser spot and frequency of 10 μm and 1 Hz, respectively. When calibrated using GBW04420 as the external standard, two samples give weighted mean 2066pb/238U ages of 504±3 Ma （2σ, n=21） and 503±3 Ma （2σ, n=22）, and only one of two samples yields a concordia U-Pb age of 507±1 Ma （2or, n=21）. These results are consistent with ID-TIMS U-Pb ages of 509±1 and 508±12 Ma and are also indistinguishable from zircon U-Pb upper intercept ages of 506±33 Ma （2σ, n=29） and 501±51 Ma （2σ, n=29）. The present study shows that in-situ U-Pb dating of uraninite can deliver more reliable formation ages of the deposit than dating coeval high-U zircon because the latter commonly suffer significant Pb loss after formation. Our results confirm that GBW04420 is an ideal matrix matching standard for in-situ U-Pb dating of uraninite.
基金supported by the National Natural Science Foundation of China(91326202,11105162,91126006,11275219)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA030104)
文摘The unique physical and chemical properties of room-temperature ionic liquids(RTILs) have recently received increasing attention as solvent alternatives for possible application in the field of nuclear industry, particularly in liquid-liquid separations of radioactive nuclides. We investigated solvent extraction of U(VI) from aqueous solutions into a commonly used ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([C4mim][NTf2]) using trioctylphosphine oxide(TOPO) as an extractant. The effects of contact time, TOPO concentration, acidity, and nitrate ions on the U(VI) extraction are discussed in detail. The extraction mechanism was proposed based on slope analysis and UV-Vis measurement. The results clearly show that TOPO/[C4mim][NTf2] provides a highly efficient extraction of U(VI) from aqueous solution under near-neutral conditions. When the TOPO concentration was 10 mmol/L, the extraction of 1 mmol/L U(VI) was almost complete(> 97%). Both the extraction efficiency and distribution coefficient were much larger than in conventional organic solvents such as dichloromethane. Slope analysis confirmed that three TOPO molecules in [C4mim][NTf2] bound with one U(VI) ion and one nitrate ion was also involved in the complexation and formed the final extracted species of [UO2(NO3)(TOPO)3]+. Such a complex suggests that extraction occurs by a cation-exchange mode, which was subsequently evidenced by the fact that the concentration of C4mim+ in the aqueous phase increased linearly with the extraction percent of U(VI) recorded by UV-Vis measurement.
