Measurement of plutonium and other actinide elements at the center for accelerator mass spectrometry: a comparative assessments of competing techniques
Low-level measurements of the long-lived actinide isotopes have a number of important applications throughout the DOE complex. These include radiobioassay programs, environmental assessments, characterization of radioactive wastes, evaluation of waste storage and treatment options, environmental remediation, basic research in chemistry and geochemistry, and other specialized non- proliferation and national security applications. As an example, it has been estimated that for the next few decades more than 1 million radiochemical analyses per year will be needed in support of US efforts to remediate the legacy of radioactive waste generated by weapons production and the nuclear power industry (Crain, 1996). Traditional radiometric counting methods do not have sufficient sensitivity to address many of these requirements. There is also a growing need to evaluate and monitor exposures to DOE workers involved in decommissioning, environmental management and/or remediation of contaminated sites and facilities. Quantitative measurements based on low-level detection techniques are of particular interest in the validation of radionuclide transport models and improving radiation dosimetry/risk estimates. Quantitative data and information are required to assess the potential health-effects of exposures occurring under special conditions (e.g., resuspension/inhalation of high-specific activity particles), of inhomogeneous radiation exposure and assessment of associated dose distributions to different parts of the body/tissue, of low dose exposure, and to validate and/or develop new and improved dosimetry models. Atom counting technology has now developed sufficiently to provide substantially better sensitivity than ionizing radiation detectors for selected long- lived radionuclides. Clearly the development of a robust, high-throughput, highly sensitive actinide measurement capability based on this new technology would have broad and sustainable impact on a range of DOE initiatives. One potential measurement technique for meeting these requirements is accelerator mass spectrometry (AMS). AMS is a widely accepted analytical technique for measurement of isotopes such as 14 C, 26 Al, 36 Cl (Vogel et al., 1995) but has only recently been demonstrated for the quantitative detection of actinides (Fifield et al., 1996). The Center for Accelerator Mass Spectrometry (CAMS) at the Lawrence Livermore National Laboratory (LLNL) operates the most versatile and most productive AMS instrument in the world (Roberts et al., 1996). The addition of a Heavy Ion Beamline and associated hardware for actinide detection are in an advanced stage of development. Detection limits for actinide elements are expected to be on the order of 1 ´ 10 6 atoms (~0.5 fg) or lower with an initial measurement capacity of a few hundred samples per year. The ultimate detection sensitivity is expected to be ~1 ´ 10 5 atoms. Here we provide a review of non-conventional measurement techniquesÑincluding AMSÑfor the determination of low-levels of 239 Pu and other actinide elements in environmental samples. We include a discussion of potential measurement interferences and sample preparation requirements for the different techniques, and outline our proposed AMS system design and strategic approach for the development of low-level actinide detection capability at CAMS.
- Research Organization:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Organization:
- USDOE Office of Defense Programs (DP)
- DOE Contract Number:
- W-7405-Eng-48
- OSTI ID:
- 7993
- Report Number(s):
- UCRL-ID-133118; HD2006400; ON: DE00007993
- Country of Publication:
- United States
- Language:
- English
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