Determination of plutonium and other transuranic elements by inductively coupled plasma mass spectrometry: A historical perspective and new frontiers in the environmental sciences |
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Authors: | Michael E. Ketterer Scott C. Szechenyi |
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Affiliation: | 1. Department of Chemistry and Biochemistry, Box 5698, Northern Arizona University, Flagstaff, AZ 86011-5698 USA;2. Department of Chemistry and Geochemistry, Colorado School of Mines, Golden, CO 80401 USA |
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Abstract: | Inductively coupled plasma mass spectrometry (ICPMS), particularly with sector field mass analyzers (SF-ICPMS), has emerged in the past several years as an excellent analytical technique for rapid, highly sensitive determination of transuranic elements (TRU) in environmental samples. SF-ICPMS has advantages of simplicity of sample preparation, high sample throughput, widespread availability in laboratories worldwide, and relatively straightforward operation when compared to other competing mass spectrometric techniques. Arguably, SF-ICPMS is the preferred technique for routine, high-throughput determination of 237Np and the Pu isotopes, excepting 238Pu, at fg-pg levels in environmental samples. Many research groups have now demonstrated the SF-ICPMS determination of 239 + 240Pu activities, 240Pu/239Pu and other Pu atom ratios in several different application areas. Many studies have examined the relative contribution of global fallout vs. local/regional Pu sources in the environment through measurement of 240Pu/239Pu and, in some cases, 241Pu/239Pu and 242Pu/239Pu. “Stratospheric fallout”, which was deposited from thermonuclear tests, conducted largely during the 1952–1964 time period, is characterized by a well-defined 240Pu/239Pu of ~ 0.18, while most other sources have different ratios. Examples of local/regional Pu sources are the Nevada Test Site, the Chernobyl plume, and accidents at Palomares, Spain and Thule, Greenland. The determination of Pu activities and atom ratios has stimulated much interest in the use of Pu as a marine tracer; several studies have shown that Pu is transported over long distances by ocean currents. 240Pu/239Pu ratios > 0.20 in sediments and seawater of the North Pacific are ascribed to ocean current transport of fallout from the Pacific Proving Ground. In nuclear forensics, much effort is focused on detection and fingerprinting of small amounts of TRU in environmental samples consisting of bulk material or individual isolated particles. Activity measurements of 239 + 240Pu, determined by SF-ICPMS, have the potential to supplement and/or replace 137Cs as a tracer of erosion, deposition, and sedimentation. Undoubtedly, the application of SF-ICPMS in TRU analysis will continue to expand, witness new developments, and generate interesting unforeseen applications in upcoming years. |
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Keywords: | AMS, accelerator mass spectrometry DC-GDMS, direct current glow discharge mass spectrometry GDMS, glow discharge mass spectrometry HASL, US Department of Energy Health and Safety Laboratory HPLC, high performance liquid chromatography IAEA, International Atomic Energy Agency ICPMS, inductively coupled plasma mass spectrometry IRMM, European Union Institute for Reference Materials and Measurements LA-ICPMS, laser ablation inductively coupled plasma mass spectrometry MC-ICPMS, multiple collector inductively coupled plasma mass spectrometry NIST, US National Institute of Standards and Technology NTS, Nevada Test Site PPG, Pacific Proving Ground Q-ICPMS, quadrupole inductively coupled plasma mass spectrometry RIMS, resonance ionization mass spectrometry SF-ICPMS, sector field inductively coupled plasma mass spectrometry SIMS, secondary ionization mass spectrometry TIMS, thermal ionization mass spectrometry TRU, transuranic elements. |
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