A paradigm shift for evaluating natural attenuation of radioactive iodine in soils and sediments: Species-specific mechanisms and pathways.

The primary approach to assessing monitored natural attenuation (MNA) is currently based on a conceptual model utilizing the total contaminant concentrations, assuming a single aqueous species. However, many contaminants, such as metals and radionuclide - including iodine, can exist in multiple species that behave chemically differently in the environment and can exist simultaneously. For example, radioiodine often occurs concurrently as three major aqueous species: iodide (I), iodate (IO), and organo-I, which undergo distinct attenuation pathways and exhibit markedly different mobility and geochemical behavior.

Spectral induced polarization of corrosion of sulfur modified Iron in sediments.

Spectral induced polarization (SIP) responses are not well understood within the context of remediation applications at contaminated sites. Systematic SIP studies are needed to gain further insights into the complex electrical response of dynamic, biogeochemical states to enable the use of SIP for subsurface site characterization and remediation monitoring. Although SIP measurements on zero valent iron have been previously published, the SIP response for sulfur modified iron (SMI), a similar potential subsurface reductive amendment, has not yet been reported.

Subsurface Transport of Plutonium in Organic and Aqueous Acidic Processing Wastes at the Hanford Site, USA.

Over 4 million liters of mixed acidic (∼pH 2.5), high ionic strength (∼5 M nitrate) plutonium (Pu) processing waste were released into the 216-Z-9 (Z-9) trench at the Hanford Site, USA, and trace Pu has migrated 37 m below the trench. In this study, we used flowthrough columns to investigate Pu transport in simplified processing waste through uncontaminated Hanford sediments to determine the conditions that led to Pu migration.

Impact of chromium (VI) as a co-contaminant on the sorption and co-precipitation of uranium (VI) in sediments under mildly alkaline oxic conditions.

Uranium (U) waste, generated at a variety of mines and nuclear production sites, migrates in the subsurface, posing a serious threat to contaminate groundwater systems. In this study, batch equilibrium and kinetic experiments, geochemical modeling and solid phase characterization were conducted to investigate the impact of Cr(VI), a common co-contaminant, on the adsorption of U(VI) to quartz, plagioclase feldspar, and carbonate-dominated sediment (≤2 mm). Batch experiments were performed under slightly alkaline conditions (7.

Review of intermediate-scale field tests in support of disposal of waste forms.

Nuclear waste has been generated from commercial nuclear reactors and from past nuclear weapons production activities. The safe disposal of this waste generally is planned to involve emplacement of packaged spent nuclear fuel (SNF) into the subsurface or reprocessing the used nuclear fuel and producing a sparingly soluble mineral or glass. The high-level waste form(s) would then be packaged and sent to a geologic repository.

Accumulation mechanisms for contaminants on weak-base hybrid ion exchange resins.

Mechanism of hexavalent chromium removal (Cr(VI) as CrO) by the weak-base ion exchange (IX) resin ResinTech® SIR-700-HP (SIR-700) from simulated groundwater is assessed in the presence of radioactive contaminants iodine-129 (as IO), uranium (U as uranyl UO), and technetium-99 (as TcO), and common environmental anions sulfate (SO) and chloride (Cl). Batch tests using the acid sulfate form of SIR-700 demonstrated Cr(VI) and U(VI) removal exceeded 97%, except in the presence of high SO concentrations (536 mg/L) where Cr(VI) and U(VI) removal decreased to ≥ 80%. However, Cr(VI) removal notably improved with co-mingled U(VI) that complexes with SO at the protonated amine sites.

Reductive removal of pertechnetate and chromate by zero valent iron under variable ionic strength conditions.

Radioactive technetium-99 (Tc) present in waste streams and subsurface plumes at legacy nuclear reprocessing sites worldwide poses potential risks to human health and environment. This research comparatively evaluated efficiency of zero-valent iron (ZVI) toward reductive removal of Tc(VII) in presence of Cr(VI) from NaCl and NaSO electrolyte solutions under ambient atmospheric conditions. In both electrolytes, anticorrosive Cr(VI) suppressed oxidation of ZVI at elevated concentrations resulting in the delay of initiation of Tc(VII) reduction to Tc(IV).

Solid phase characterization and transformation of illite mineral with gas-phase ammonia treatment.

In situ remediation applications of ammonia (NH) gas have potential for sequestration of subsurface contamination. Ammonia gas injections initially increase the pore water pH leading to mineral dissolution followed by formation of secondary precipitates as the pH is neutralized. However, there is a lack of understanding of fundamental alteration processes due to NH treatment.

Time dependent zero valent iron oxidation and the reductive removal of pertechnetate at variable pH.

Elemental iron Fe is a promising reductant for removal of radioactive technetium-99 (Tc) from complex aqueous waste streams that contain sulfate, halides, and other inorganic anions generated during processing of legacy radioactive waste. The impact of sulfate on the kinetics of oxidation and reduction capacity of Fe in the presence of Tc has not been examined. We investigated the oxidative transformation of Fe and reductive removal of TcO in 0.

Spontaneous redox continuum reveals sequestered technetium clusters and retarded mineral transformation of iron.

The sequestration of metal ions into the crystal structure of minerals is common in nature. To date, the incorporation of technetium(IV) into iron minerals has been studied predominantly for systems under carefully controlled anaerobic conditions. Mechanisms of the transformation of iron phases leading to incorporation of technetium(IV) under aerobic conditions remain poorly understood.

In situ reductive dissolution to remove Iodine-129 from aquifer sediments.

The use of an aqueous reductant (Na-dithionite) with pH buffer (K-carbonate, pH 12) was evaluated in this laboratory study as a potential remedial approach for removing Fe oxide associated iodine and enhancing pump-and-treat extraction from iodine-contaminated sediments in the unconfined aquifer in the 200 West Area of the Hanford Site. X-ray fluorescence data of untreated sediment indicated that iodine was largely associated with Fe (i.e.

Comparative analysis of ZVI materials for reductive separation of Tc(VII) from aqueous waste streams.

Technetium-99 (Tc) is a long-lived radioactive contaminant present in legacy nuclear waste streams and contaminated plumes of the nuclear waste storage sites worldwide that poses risks for human health and the environment. Pertechnetate (TcO), the most common chemical form of Tc under oxidative conditions, is of particular concern due to its high aqueous solubility and mobility in the subsurface. One approach to treatment and remediation of TcO is reduction of Tc to less soluble and mobile Tc and its removal from the contaminated streams such as liquid secondary waste generated during vitrification of the Hanford low activity tank waste.

Potential for U sequestration with select minerals and sediments via base treatment.

Temporary base treatment is a potential remediation technique for heavy metals through adsorption, precipitation, and co-precipitation with minerals. Manipulation of pH with ammonia gas injection may be especially useful for vadose zone environments as it does not require addition of liquids that would increase the flux towards groundwater. In this research, we conducted laboratory batch experiments to evaluate the changes in uranium mobility and mineral dissolution with base treatments including sodium hydroxide, ammonium hydroxide, and ammonia gas.

Effects of ammonium on uranium partitioning and kaolinite mineral dissolution.

Ammonia gas injection is a promising technique for the remediation of uranium within the vadose zone. It can be used to manipulate the pH of a system and cause co-precipitation processes that are expected to remove uranium from the aqueous phase and decrease leaching from the solid phase. The work presented in this paper explores the effects of ammonium and sodium hydroxide on the partitioning of uranium and dissolution of the kaolinite mineral in simplified synthetic groundwaters using equilibrium batch sorption and sequential extraction experiments.

Experimental evidence for ternary colloid-facilitated transport of Th(IV) with hematite (α-FeO) colloids and Suwannee River fulvic acid.

Previous field experiments have suggested colloid-facilitated transport via inorganic and organic colloids as the primary mechanism of enhanced actinide transport in the subsurface at former nuclear weapons facilities. In this work, research was guided by the hypothesis that humic substances can enhance tetravalent actinide (An(IV)) migration by coating and mobilizing natural colloids in environmental systems and increasing An(IV) sorption to colloids. This mechanism is expected to occur under relatively acidic conditions where organic matter can sorb and coat colloid surfaces and facilitate formation of ternary colloid-ligand-actinide complexes.

Impact of bottled water storage duration and location on bacteriological quality.

An investigation studying the effects of storage duration and location on the persistence of heterotrophic microorganisms in oligotrophic bottled water environments has been completed. One-gallon high-density polyethylene water containers stored for up to 16 weeks at temperatures ranging from 2°C to >49°C in a refrigerator, indoor cabinet, covered porch, and car trunk were evaluated for microbiological quality. Heterotrophic plate counts (HPCs) of up to 4 × 10(3) cfu/mL were detected in containers stored on a porch and car trunk; whereas, HPCs were found not to exceed 400 cfu/mL and 100 cfu/mL for bottles stored in indoor cabinets and refrigerators, respectively.