Brian Patrick Spalding

In Situ Bioremediation of Uranium with Emulsified Vegetable Oil as the Electron Donor

A field test with a one-time emulsified vegetable oil (EVO) injection was conducted to assess the capacity of EVO to sustain uranium bioreduction in a high-permeability gravel layer with groundwater concentrations of (mM) U, 0.0055; Ca, 2.98; NO3(-), 0.11; HCO3(-), 5.07; and SO4(2-), 1.23. Comparison of bromide and EVO migration and distribution indicated that a majority of the injected EVO was retained in the subsurface from the injection wells to 50 m downgradient. Nitrate, uranium, and sulfate were sequentially removed from the groundwater within 1-2 weeks, accompanied by an increase in acetate, Mn, Fe, and methane concentrations. Due to the slow release and degradation of EVO with time, reducing conditions were sustained for approximately one year, and daily U discharge to a creek, located approximately 50 m from the injection wells, decreased by 80% within 100 days. Total U discharge was reduced by 50% over the one-year period. Reduction of U(VI) to U(IV) was confirmed by synchrotron analysis of recovered aquifer solids. Oxidants (e.g., dissolved oxygen, nitrate) flowing in from upgradient appeared to reoxidize and remobilize uranium after the EVO was exhausted as evidenced by a transient increase of U concentration above ambient values. Occasional (e.g., annual) EVO injection into a permeable Ca and bicarbonate-containing aquifer can sustain uranium bioreduction/immobilization and decrease U migration/discharge.

Distribution and relationship of radionuclides to streambed gravels in a small watershed

In White Oak Creek watershed in eastern Tennessee, the radionuclides60Co,90Sr, and137Cs were retained by streambed gravels on different sites:60Co was associated with manganese in the hydrous oxide coatings on rocks and minerals;90Sr occurred primarily as an exchangeable cation although small amounts were held in a nonexchangeable form; and137Cs was held very selectively, presumably by illite in shale fragments composing the sediment. The distribution of radionuclides on sediments was size dependent: the 0.85–3.35 mm fine-gravel fraction was higher in radionuclide concentration than the sand fraction. An areal survey of radionuclide concentrations on streambed gravels from throughout the watershed, located numerous contamination sources. These radionuclide concentrations, when combined with both distribution coefficients of radionuclides between gravel and water and drainage area, were used to rank subsections of the watershed by their relative contribution to the overall contamination of the watershed. For90Sr, this ranking procedure agreed with the measured discharges of subsections of the watershed which are routinely monitored.

Volatilization of Cesium-137 from Soil with Chloride Amendments during Heating and Vitrification.

During vitrification of soil and soil:limestone mixtures, significant volatilization (> 10%) of the radioisotope [sup 137]Cs occurred particularly in the presence of small amounts ( 99% of the [sup 137]Cs by repeated amendment and treatment at 1000[degree]C. Amendment with sodium borate and subsequent heating to 1200[degree]C also stimulated significant volatilization of [sup 137]Cs. However, amendments up to 10% of other chemicals including carbonates, nitrates, phosphates, sulfates, fluorides, polystyrene, graphite, stainless steels, iron, zinc oxide, and antimony oxide did not increase [sup 137]Cs volatilization compared to unamended samples. The majority of the chloride-induced volatilization occurred between 800 and 1000[degree]C for sodium chloride-amended samples of both soil and soil:limestone mixtures. Thus, an effective and potentially efficient soil decontamination technique for [sup 137]Cs has been identified. 17 refs., 8 figs., 3 tabs.

Hydrogel-Encapsulated Soil: A Tool to Measure Contaminant Attenuation In Situ

Hydrogel encapsulation presents a novel and powerful general method to observe many water-solid contaminant interactions in situ for a variety of aqueous media including groundwater, with a variety of nondestructive analytical methods, and with a variety of solids including contaminated soil. After intervals of groundwater immersion, polyacrylamide hydrogel-encapsulated solid specimens were retrieved, assayed nondestructively for uranium and other elements using X-ray fluorescence spectroscopy, and replaced in groundwater for continued reaction. Desorption dynamics of uranium from contaminated soils and other solids, when moved to uncontaminated groundwater, were fit to a general two-component kinetic retention model with slow-release and fast-release fractions for the total uranium. In a group of Oak Ridge soils with varying ambient uranium contamination (169-1360 mg/kg), the uranium fraction retained under long-term in situ kinetic behavior was strongly correlated (r(2) = 0.89) with residual uranium after laboratory sequential extraction of water-soluble and cation-exchangeable fractions of the soils. To illustrate how potential remedial techniques can be compared to natural attenuation, thermal stabilization of one soil increased the size of its long-term in situ retained fraction from 50% to 88% of the total uranium and increased the half-life of that long-term retained fraction from 990 to 40000 days.