Inductively coupled plasma-sector field mass spectrometry with a high-efficiency sample introduction system for the determination of Pu isotopes in settling particles at femtogram levels.

An analytical method for the determination of plutonium concentration and its isotope ratio ((240)Pu/(239)Pu) for settling particle samples by inductively coupled plasma mass spectrometry (ICP-MS) is presented. The generally used approach for Pu preconcentration by increasing the amount of samples is not applicable because of the small size of settling particle samples available for the analysis for Pu isotopes. Efforts were made to improve the sensitivity of a sector-field ICP-MS (SF-ICP-MS) and reduce the (238)UH(+) interference for Pu analysis by combining a high-efficiency sample introduction system (APEX-Q). An extremely low detection limit of 0.07 fg Pu was achieved, which allowed the determination of Pu isotope ratio at femtogram levels. The precision and accuracy of (240)Pu/(239)Pu isotope ratio analysis were carefully examined with a certified Pu isotope standard (NBS-947) and an ocean sediment reference material (IAEA-368). Simple anion-exchange chromatography for the separation and purification of Pu was combined with the APEX-Q/SF-ICP-MS system to determine Pu isotopes in settling particles collected in the East China Sea continental margin. The obtained results supported a previous observation on the lateral transport of Pu containing particles in this continental margin.

[1]  R. Chiappini,et al.  Development of a high-sensitivity inductively coupled plasma mass spectrometer for actinide measurement in the femtogram range , 1996 .

[2]  P. Povinec,et al.  The development of sequential separation methods for the analysis of actinides in sediments and biological materials using anion-exchange resins and extraction chromatography , 2005 .

[3]  G. Hong,et al.  Plutonium isotopes in seas around the Korean Peninsula. , 2004, The Science of the total environment.

[4]  S. Uchida,et al.  Determination of plutonium concentration and its isotopic ratio in environmental materials by ICP-MS after separation using and extraction chromatography , 1999 .

[5]  T. Aono,et al.  Determination of plutonium and its isotopic ratio in marine sediment samples using quadrupole ICP-MS with the shield torch system under normal plasma conditions , 2004, Analytical and bioanalytical chemistry.

[6]  J. Stannard Plutonium in the Environment , 1973 .

[7]  Kunjai Lee,et al.  Rapid determination of Pu isotopes and atom ratios in small amounts of environmental samples by an on-line sample pre-treatment system and isotope dilution high resolution inductively coupled plasma mass spectrometry , 2000 .

[8]  R. Scott,et al.  The measurement of the isotopic composition of plutonium in an Irish Sea sediment by mass spectrometry , 1995 .

[9]  Masatoshi Yamada,et al.  Vertical distributions of 239+240Pu activities and 240Pu/239Pu atom ratios in sediment cores: implications for the sources of Pu in the Japan Sea. , 2005, The Science of the total environment.

[10]  J. Becker State-of-the-art and progress in precise and accurate isotope ratio measurements by ICP-MS and LA-ICP-MS , 2002 .

[11]  G. Hong,et al.  240Pu/239Pu atom ratios in the bottom sediments of the NW Pacific Ocean , 2003 .

[12]  Masatoshi Yamada,et al.  Plutonium activities and 240Pu/239Pu atom ratios in sediment cores from the east China sea and Okinawa Trough: Sources and inventories , 2005 .

[13]  A. J. Walder,et al.  Validation of the analytical linearity and mass discrimination correction model exhibited by a multiple collector inductively coupled plasma mass spectrometer by means of a set of synthetic uranium isotope mixtures , 1995 .

[14]  H. Higuchi,et al.  Concentration of plutonium in squids collected from Japanese inshore measured by HR-ICP-MS, 1981–2000 , 2002 .

[15]  Masatoshi Yamada,et al.  Sediment core record of global fallout and Bikini close-in fallout Pu in Sagami Bay, Western Northwest Pacific margin. , 2004, Environmental science & technology.

[16]  Ken O. Buesseler,et al.  The isotopic signature of fallout plutonium in the North Pacific , 1997 .

[17]  D. Fisher,et al.  Direct determination of lead isotopes (206Pb, 207Pb, 208Pb) in arctic ice samples at picogram per gram levels using inductively coupled plasma-sector field MS coupled with a high-efficiency sample introduction system. , 2004, Analytical chemistry.

[18]  K. Heumann,et al.  Precision and accuracy in isotope ratio measurements by plasma source mass spectrometry , 1998 .

[19]  Gi Hoon Hong,et al.  Distribution and inventories of 90Sr, 137Cs, 241Am and Pu isotopes in sediments of the Northwest Pacific Ocean , 2005 .

[20]  P. Masqué,et al.  The role of sea ice in the fate of contaminants in the Arctic Ocean: plutonium atom ratios in the Fram Strait. , 2003, Environmental science & technology.

[21]  Kunjai Lee,et al.  Determination of pu isotopes in seawater by an on-line sequential injection technique with sector field inductively coupled plasma mass spectrometry. , 2002, Analytical chemistry.

[22]  T. Aono,et al.  Large particle flux of 239+240Pu on the continental margin of the East China Sea. , 2002, The Science of the total environment.

[23]  Chih-An Huh,et al.  Sedimentation in the Southern Okinawa Trough: enhanced particle scavenging and teleconnection between the Equatorial Pacific and western Pacific margins , 2004 .

[24]  M. Yamada,et al.  Determination of U isotope ratios in sediments using ICP-QMS after sample cleanup with anion-exchange and extraction chromatography. , 2006, Talanta.

[25]  P. Santschi,et al.  The 129iodine bomb pulse recorded in Mississippi River Delta sediments: results from isotopes of I, Pu, Cs, Pb, and C , 2000 .

[26]  J. Grebmeier,et al.  Sources of the transuranic elements plutonium and neptunium in arctic marine sediments , 2000 .

[27]  R. Anderson,et al.  Determination of natural actinides and plutonium in marine particulate material , 1982 .

[28]  J. Mietelski,et al.  Resolving global versus local/regional Pu sources in the environment using sector ICP-MS , 2004 .

[29]  M. Yamada,et al.  Postdepositional enrichment of uranium in sediment from the Bering Sea , 1984 .

[30]  V. T. Bowen,et al.  Fallout radionuclides in the Pacific Ocean: Vertical and horizontal distributions, largely from GEOSECS stations , 1980 .