Hydrologic and geochemical controls on the transport of radionuclides in natural undisturbed arid environments as determined by accelerator mass spectrometry measurements
This project developed techniques for measuring globally distributed radionuclides that occur today in extremely low abundances (''fallout'' from the era of atmospheric nuclear testing), and then applied these techniques to better understand the mechanisms by which radionuclides migrate. The techniques employ accelerator mass spectrometry (AMS), a relatively new analytical tool that permits this work to be conducted for the first time. The goal in this project was to develop AMS analytical techniques for {sup 129}I (fallout concentration: {approx} 10{sup 6} atoms/g) {sup 99}Tc ({approx} 10{sup 9} atoms/g), {sup 90}Sr ({approx}10{sup 7} atoms/gram soil), and {sup 93}Zr ({approx} 10{sup 9} atoms/g), and improved methods for {sup 36}Cl ({approx} 10{sup 9} atoms/g). As a demonstration of the analytical techniques, and as an investigation of identified problems associated with characterizing moisture and radionuclide movement in unsaturated desert soils, we developed a vadose zone research site at the Nevada Test Site. Our findings can be summarized as follows: (1) The distribution of chloride and {sup 36}Cl at the research site indicates that the widely-used ''chloride accumulation'' method for estimating moisture flux is erroneous; some mechanism for attenuation of chloride exists, violating an assumption of the accumulation method; (2) {sup 129}I is fractionated into several soil compartments that have varying migration abilities; the two most mobile can be tentatively identified as Fe/Mn oxyhydroxides and organic acids based on our sequential leaching techniques; (3) These most mobile constituents are capable of migrating at a rate greater than that of {sup 36}Cl, usually considered the most mobile solute in hydrologic systems; these constituents may be colloidal in character, of neutral surface charge, and therefore conservative in aqueous migration; (4) {sup 99}Tc is readily measurable by AMS, as we demonstrate by the first AMS {sup 99}Tc measurements of contaminated waters; extraction of {sup 99}Tc from silicate soils is difficult, but can be done using the extended methods we have developed; (5 ) Most of the bomb-pulse {sup 99}Tc observed in the soil profile at the EMSP research site was confined to the upper 50 cm; however, there is some indication that a fraction of the {sup 99}Tc could move to the same extent as bomb-pulse {sup 36}Cl; and (6) The observed AMS sensitivity for {sup 90}Sr was {sup 90}Sr/Sr=10{sup -12}, corresponding to about 20-200 mBq per sample, similar to the sensitivity of traditional decay counting; further work should improve the sensitivity by at least a factor of 10, but even now the AMS ability for sensitive, high throughput, fast turnaround, robust measurements using simple chemistry is an improvement over decay counting methods. Although our results regarding the migration of these radionuclides in arid soils increase the scientific understand of contaminant migration in that environment, we believe the primary benefit of our EMSP research is the development of AMS analytical techniques for low-level radionuclide measurement. The advantages of this include: (1) the ability to conduct migration studies in locations most like those of concern to public health, e.g., a ''far-field'' environment; (2) sites of multiple contamination, e.g., by VOC's, can be avoided; (3) it becomes unnecessary to collect research samples that are themselves radioactive waste and are therefore difficult to handle and dispose of in the laboratory; and (4) since the nuclides are globally distributed, migration research can be conducted in any chosen environment. Our research is therefore designed to make the study of radionuclide migration simpler to do, simpler to interpret, and easier to apply to specific DOE sites. This will lead to a better understanding of the migration potential and ultimate fate of radionuclides, creating much less uncertainty regarding which remediative strategies should be employed. For any project, this will reduce its cost, shorten its schedule, and provide greater confidence in its final result, both for the DOE and for the general public. We feel this is a substantial contribution to the EM community.
- Research Organization:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- W-7405-ENG-48
- OSTI ID:
- 15013403
- Report Number(s):
- UCRL-ID-133321; TRN: US0600847
- Country of Publication:
- United States
- Language:
- English
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