Effective half-life of caesium-137 in various environmental media at the Savannah river site.

During the operational history of the Savannah River Site (SRS), many different radionuclides have been released from site facilities into the SRS environment. However, only a relatively small number of pathways, most importantly (137)Cs in fish and deer, have contributed significantly to doses and risks to the public. The "effective" half-lives (Te) of (137)Cs (which include both physical decay and environmental dispersion) in Savannah River floodplain soil and vegetation and in fish and white-tailed deer from the SRS were estimated using long-term monitoring data. For 1974-2011, the Tes of (137)Cs in Savannah River floodplain soil and vegetation were 17.0 years (95% CI = 14.2-19.9) and 13.4 years (95% CI = 10.8-16.0), respectively. These Tes were greater than in a previous study that used data collected only through 2005 as a likely result of changes in the flood regime of the Savannah River. Field analyses of (137)Cs concentrations in deer collected during yearly controlled hunts at the SRS indicated an overall Te of 15.9 years (95% CI = 12.3-19.6) for 1965-2011; however, the Te for 1990-2011 was significantly shorter (11.8 years, 95% CI = 4.8-18.8) due to an increase in the rate of (137)Cs removal. The shortest Tes were for fish in SRS streams and the Savannah River (3.5-9.0 years), where dilution and dispersal resulted in rapid (137)Cs removal. Long-term data show that Tes are significantly shorter than the physical half-life of (137)Cs in the SRS environment but that they can change over time. Therefore, it is desirable have a long period of record for calculating Tes and risky to extrapolate Tes beyond this period unless the processes governing (137)Cs removal are clearly understood.

Changes in 137Cs concentrations in soil and vegetation on the floodplain of the Savannah River over a 30 year period.

(137)Cs released during 1954-1974 from nuclear production reactors on the Savannah River Site, a US Department of Energy nuclear materials production site in South Carolina, contaminated a portion of the Savannah River floodplain known as Creek Plantation. (137)Cs activity concentrations have been measured in Creek Plantation since 1974 making it possible to calculate effective half-lives for (137)Cs in soil and vegetation and assess the spatial distribution of contaminants on the floodplain. Activity concentrations in soil and vegetation were higher near the center of the floodplain than near the edges as a result of frequent inundation coupled with the presence of low areas that trapped contaminated sediments. (137)Cs activity was highest near the soil surface, but depth related differences diminished with time as a likely result of downward diffusion or leaching. Activity concentrations in vegetation were significantly related to concentrations in soil. The plant to soil concentration ratio (dry weight) averaged 0.49 and exhibited a slight but significant tendency to decrease with time. The effective half-lives for (137)Cs in shallow (0-7.6 cm) soil and in vegetation were 14.9 (95% CI=12.5-17.3) years and 11.6 (95% CI=9.1-14.1) years, respectively, and rates of (137)Cs removal from shallow soil and vegetation did not differ significantly among sampling locations. Potential health risks on the Creek Plantation floodplain have declined more rapidly than expected on the basis of radioactive decay alone because of the relatively short effective half-life of (137)Cs.

Interactions among phosphate amendments, microbes and uranium mobility in contaminated sediments.

The use of sequestering agents for the transformation of radionuclides in low concentrations in contaminated soils/sediments offers considerable potential for environmental cleanup. This study evaluated the influence of three types of phosphate (rock phosphate, biological phosphate, and calcium phytate) and two microbial amendments (Alcaligenes piechaudii and Pseudomonas putida) on U mobility. All tested phosphate amendments reduced aqueous U concentrations more than 90%, likely due to formation of insoluble phosphate precipitates. The addition of A. piechaudii and P. putida alone were found to reduce U concentrations 63% and 31%, respectively. Uranium removal in phosphate treatments was significantly reduced in the presence of the two microbes. Two sediments were evaluated in experiments on the effects of phosphate amendments on U mobility, one from a stream on the Department of Energy's Savannah River Site near Aiken, SC and the other from the Hanford Site, a Department of Energy facility in Washington state. Increased microbial activity in the treated sediment led to a reduction in phosphate effectiveness. The average U concentration in 1 M MgCl(2) extract from U contaminated sediment was 437 microg/kg, but in the same sediment without microbes (autoclaved), the extractable U concentration was only 103 microg/kg. The U concentration in the 1 M MgCl(2) extract was approximately 0 microg/kg in autoclaved amended sediment treated with autoclaved biological apatite. These results suggest that microbes may reduce phosphate amendment remedial effectiveness.

Long-term changes in mercury concentrations in fish from the middle Savannah River.

Total mercury levels were measured in largemouth bass (Micropterus salmoides), "sunfish" (Lepomis spp.), and "catfish" (primarily Ameiurus spp. and Ictalurus punctatus) from 1971 to 2004 in the middle Savannah River (river km 191 to 302), which drains the coastal plain of the southeastern U.S. Total mercury concentrations were higher in largemouth bass (overall mean of 0.55 mg/kg from 1971 to 2004), a piscivorous (trophic level 4) species than in the other taxa (means of 0.22-0.26 mg/kg), but temporal trends were generally similar among taxa. Mercury levels were highest in 1971 but declined over the next 10 years due to the mitigation of point source industrial pollution. Mercury levels in fish began to increase in the 1980s as a likely consequence of mercury inputs from tributaries and associated wetlands where mercury concentrations were significantly elevated in water and fish. Mercury levels in Savannah River fish decreased sharply in 2001-2003 coincident with a severe drought in the Savannah River basin, but returned to previous levels in 2004 with the resumption of normal precipitation. Regression models showed that mercury levels in fish changed significantly over time and were affected by river discharge. Mercury levels in Savannah River fish were only slightly lower in 2004 (0.3 to 0.8 mg/kg) than in 1971 (0.4 to 1.0 mg/kg) despite temporal changes during the intervening years.

Phosphate sources and their suitability for remediation of contaminated soils.

Phosphate minerals and specifically apatite show promise for environmental cleanup because they can form stable compounds with a wide range of cationic contaminants. However, phosphate minerals naturally accumulate some heavy metals that may cause additional contamination of the environment if used improperly. Nine commercially available phosphate materials were evaluated for remediation of contaminated soil based on solubility, concentration of metal/metalloid impurities, and leachability of impurity metal/metalloids. The phosphate materials consisted of three groups: processed (i.e., fertilizers), mined (rock phosphates from different formations), and biogenic (ground fish bone). Processed and mined rock phosphates contained relatively high total concentrations of As, Co, Cr, and Cu but did not exceed the RCRA toxicity characteristic leaching procedure (TCLP) limits. Biogenic apatite contained much lower metal concentrations than processed and mined rock phosphate and was appreciably more soluble. By combining biogenic and mined phosphate it is possible to obtain a wide range of phosphate release rates, permitting rapid immobilization of contaminants while providing a slow release of phosphate for continued long-term treatment.

Potential of largemouth bass as vectors of 137Cs dispersal.

We conducted a radio telemetry study on the movements of potentially contaminated largemouth bass between Steel Creek, a restricted access (137)Cs contaminated stream on the Savannah River Site (located in South Carolina, USA), and the publicly accessible Savannah River. Largemouth bass were relatively mobile in lower Steel Creek and the portion of the Savannah River near Steel Creek, and there was considerable movement between these two habitats. Largemouth bass had home ranges of about 500 linear meters of shoreline in the Savannah River but sometimes moved long distances. Such movements occurred primarily during the spawning season, largely upstream, and increased when water levels were changing or elevated. However, approximately 90% of the largemouth bass observations were within 10 km of Steel Creek. The total quantity of (137)Cs transported into the Savannah River by largemouth bass was much less than transported by water and suspended sediments discharged from Steel Creek. We conclude that largemouth bass from the Savannah River Site are unlikely to be responsible for long distance dispersal of substantial radiological contamination in the Savannah River.

Influence of methylmercury from tributary streams on mercury levels in Savannah River Asiatic clams.

Average methylmercury levels in five Savannah River tributary streams, sampled 11 times over 2 years (0.170 ng/l), were nearly twice as high as in the Savannah River (0.085 ng/l). Total mercury levels in the tributaries (2.98 ng/l) did not differ significantly from the river (2.59 ng/l). All of the tributaries drained extensive wetlands that would be expected to support comparatively high rates of methylation. Mercury concentrations in Asiatic clams (Corbicula fluminea) collected from the discharge plumes of Savannah River tributaries (average of 0.044 microg/g wet weight) were significantly (P<0.001) higher than in Asiatic clams collected from the Savannah River upstream from the tributary mouths (average of 0.017 microg/g wet weight). These results indicate that streams draining wetlands into coastal plain rivers can create localized areas of elevated methylmercury with resulting increases in the mercury levels of river biota.

Influences on mercury bioaccumulation factors for the Savannah River.

Mercury TMDLs (Total Maximum Daily Loads) are a regulatory instrument designed to reduce the amount of mercury entering a water body and ultimately to control the bioaccumulation of mercury in fish. TMDLs are based on a BAF (bioaccumulation factor), which is the ratio of methyl mercury in fish to dissolved methyl mercury in water. Analysis of fish tissue and aqueous methyl mercury samples collected at a number of locations and over several seasons in a 118-km reach of the Savannah River demonstrated that species-specific BAFs varied by factors of three to eight. Factors contributing to BAF variability were location, habitat, and season-related differences in fish muscle tissue mercury levels and seasonal differences in dissolved methyl mercury levels. Overall (all locations, habitats, and seasons) average BAFs were 3.7 x 10(6) for largemouth bass, 1.4 x 10(6) for sunfishes, and 2.5 X 10(6) for white catfish. Determination of representative BAFs for mercury in fish from large rivers necessitates collecting large and approximately equal numbers of fish and aqueous methyl mercury samples over a seasonal cycle from the entire area and all habitats to be represented by the TMDL.

Ecological half-lives of 137Cs in fishes from the Savannah River Site.

Ecological half-lives (Te's) were estimated for 137Cs in largemouth bass, sunfishes, and bullheads from two reservoirs and three streams on the Savannah River Site, a nuclear weapons material production facility in South Carolina. Ecological half-life is the time required for a given contaminant concentration to decrease by 50% as a result of physical, chemical, and/or biological processes that remove it from an ecosystem or render it biologically unavailable. Te's were estimated from whole-fish 137Cs concentrations in samples collected during 1972-1996, following radionuclide releases that occurred primarily during the 1960's and early 1970's. Te's ranged from 3.2 to 16.7 y, and all were shorter than expected from the half-life for radioactive decay (Tp = 30.2 y) alone. Fish taxa from the same locations differed in mean 137Cs concentrations (highest in largemouth bass and lowest in sunfishes) but, in most cases, exhibited similar 137Cs Te's. Rates of 137Cs removal in fishes were strongly correlated with rates of 137Cs removal in water. The shortest Te's occurred in the upper portions of the streams. Te's in lower portions of the streams were longer, as were Te's in one of the reservoirs. Te's in the second reservoir, which had a much shorter water residence time, were nearly comparable to those in the upper portions of the streams until 1991. At that time, 137Cs concentrations in fishes began to increase following drainage and refilling of the reservoir, which apparently resuspended 137Cs buried in the sediments.