Biogeochemical Processes Responsible for the Enhanced Transport of Plutonium Under transient Unsaturated Ground Water Conditions
To better understand longer-term vadose zone transport in southeastern soils, field lysimeter experiments were conducted at the Savannah River Site (SRS) near Aiken, SC, in the 1980s. Each of the three lysimeters analyzed herein contained a filter paper spiked with different Pu solutions, and they were left exposed to natural environmental conditions (including the growth of annual weed grasses) for 11 years. The resulting Pu activity measurements from each lysimeter core showed anomalous activity distributions below the source, with significant migration of Pu above the source. Such results are not explainable by adsorption phenomena alone. A transient variably saturated flow model with root water uptake was developed and coupled to a soil reactive transport model. Somewhat surprisingly, the fully transient analysis showed results nearly identical to those of a much simpler steady flow analysis performed previously. However, all phenomena studied were unable to produce the upward Pu transport observed in the data. This result suggests another transport mechanism such as Pu uptake by roots and upward transport due to transpiration. Thus, the variably saturated flow and reactive transport model was extended to include uptake and transport of Pu within the root xylem, along with computational methodology and results. In the extended model, flow velocity in the soil was driven by precipitation input along with transpiration and drainage. Water uptake by the roots determined the flow velocity in the root xylem, and this along with uptake of Pu in the transpiration stream drove advection and dispersion of the two Pu species in the xylem. During wet periods with high potential evapotranspiration, maximum flow velocities through the xylem would approached 600 cm/hr, orders of magnitude larger that flow velocities in the soil. Values for parameters and the correct conceptual viewpoint for Pu transport in plant xylem was uncertain. This motivated further experiments devoted to Pu uptake by corn roots and xylem transport. Plants were started in wet paper wrapped around each corn seed. When the tap roots were sufficiently long, the seedlings were transplanted to a soil container with the tap root extending out the container bottom. The soil container was then placed over a nutrient solution container, and the solution served as an additional medium for root growth. To conduct an uptake study, a radioactive substance, such as Pu complexed with the bacterial siderophore DFOB, was added to the nutrient solution. After a suitable elapsed time, the corn plant was sacrificed, cut into 10 cm lengths, and the activity distribution measured. Experimental results clarified the basic nature of Pu uptake and transport in corn plants, and resulting simulations suggested that each growing season Pu in the SRS lysimeters would move into the plant shoots and be deposited on the soil surface during the Fall dieback. Subsequent isotope ratio analyses showed that this did happen. OVERALL RESULTS AND CONCLUSIONS - (1) Pu transport downward from the source is controlled by advection, dispersion and adsorption, along with surface-mediated REDOX reactions. (2) Hysteresis, extreme root distribution functions, air-content dependent oxidation rate constants, and large evaporation rates from the soil surface were not able to explain the observed upward migration of Pu. (3) Small amounts of Pu uptake by plant roots and translocation in the transpiration stream creates a realistic mechanism for upward Pu migration (4) Realistic xylem cross-sectional areas imply high flow velocities under hot, wet conditions. Such flow velocities produce the correct shape for the observed activity distributions in the top 20 cm of the lysimeter soil. (5) Simulations imply that Pu should have moved into the above-ground grass tissue each year during the duration of the experiments, resulting in an activity residual accumulating on the soil surface. An isotope ratio analysis showed that the observed surface Pu residue was from the buried sources, not atmospheric fallout. (6) The plant experiments indicate a Pu-DFOB velocity in the corn xylem of at least 174 cm/hr, much higher than ionic Pu in soil. Thus, Pu complexation with chelating agents is probably what led to the observed enhanced uptake and mobility in grasses. (7) Plant experiments show that the uptake of Fe-DFOB, Pu-DFOB and the resulting distributions are very similar. This supports the hypothesis that plant and bacterial iron-seeking chemistry mistakes Pu for Fe.
- Research Organization:
- Clemson Univ., SC (United States)
- Sponsoring Organization:
- DOE Office of Science, Chicago Office
- DOE Contract Number:
- FG02-07ER64401
- OSTI ID:
- 979900
- Report Number(s):
- DOE-ER-64401; TRN: US1200182
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
54 ENVIRONMENTAL SCIENCES
CHELATING AGENTS
CONTAINERS
DISTRIBUTION FUNCTIONS
FLOW MODELS
GROUND WATER
ISOTOPE RATIO
LYSIMETERS
NUTRIENTS
OXIDATION
PLUTONIUM
REDOX REACTIONS
STEADY FLOW
TRANSIENTS
TRANSPIRATION
TRANSPORT
VELOCITY
WATER
plutonium
transport
vadose zone
biochemical
redox