Determination of plutonium and other transuranic elements by inductively coupled plasma mass spectrometry: A historical perspective and new frontiers in the environmental sciences

作者：Ketterer Michael E^*; Szechenyi Scott C

来源：Spectrochimica Acta Part B: Atomic Spectroscopy , 2008, 63(7): 719-737.

DOI：10.1016/j.sab.2008.04.018

• transuranic elements
• environment
• ICPMS
• marine tracer
• earth/environmental processes

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 Np-237 and the Pu isotopes, excepting Pu-238, at fg-pg levels in environmental samples. Many research groups have now demonstrated the SF-ICPMS determination of Pu239+240 activities Pu-240/Pu-239 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 Pu-240/ Pu-239 and, in some cases, Pu-241/Pu-239 and Pu-242/Pu-239. "Stratospheric fallout", which was deposited from thermonuclear tests, conducted largely during the 1952-1964 time period, is characterized by a well-defined Pu-240/Pu-239 of similar to 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. Pu-240/Pu-239 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 Pu239+240, determined by SF-ICPMS, have the potential to supplement and/or replace Cs-137 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.

• 出版日期2008-7