Flux Crystal Growth of the Extended Structure Pu(V) Borate Na(PuO)(BO).

As part of our exploration of plutonium-containing materials as potential nuclear waste forms, we report the first extended structure Pu(V) material and the first Pu(V) borate. Crystals of Na(PuO)(BO) were grown out of mixed hydroxide/boric acid flux and found to crystallize in the orthorhombic space group with lattice parameters of = 9.9067(4) Å, = 6.

Proton nuclear magnetic resonance (1H NMR) of flammable organic chemicals in radioactive high-level supernatant waste at the Savannah River Site (SRS).

The Savannah River Site stores approximately 36 million gallons of radioactive and hazardous waste that contains approximately 245 million curies. The waste is sent through various chemical processes to reduce its volume and to separate various components. The facility plans to replace formic acid (a chemical used to reduce soluble mercury) with glycolic acid.

Developing Waste Forms for Transuranic Elements: Quaternary Neptunium Fluorides of the Type NaMNpF (M = Ti, V, Cr, Mn, Fe, Co, Ni, Al, Ga).

A series of quaternary Np(IV) fluorides was synthesized using a mild hydrothermal synthesis approach. The compositions are all of the type NaMNpF, where M = Ti(III), V(III), Cr(III), Mn(II), Fe(III), Co(II), Ni(II), Al(III), and Ga(III) and = 4 for divalent metals, = 3 for trivalent metals. The compounds all crystallize in the -31 space group and are isotypic with actinide analogues NaMAnF (An = Ce, U, Th, Pu).

PLA Renewable Bio Polymer Based Solid-State Gamma Radiation Detector-Dosimeter for Biomedical and Nuclear Industry Applications.

Polylactic acid (PLA) as a "green," renewable corn-soy based polymer resin was assessed as a novel solid-state detector for rapid-turnaround gamma radiation dosimetry in the 1-100 kGy range-of significant interest in biomedical and general nuclear industry applications. Co-60 was used as the source of gamma photons. It was found that PLA resin responds well in terms of rheology and porosity metrics with an absorbed gamma dose (Dg).

Capture Instead of Release: Defect-Modulated Radionuclide Leaching Kinetics in Metal-Organic Frameworks.

Comparison of defect-controlled leaching-kinetics modulation of metal-organic frameworks (MOFs) and porous functionalized silica-based materials was performed on the example of a radionuclide and radionuclide surrogate for the first time, revealing an unprecedented readsorption phenomenon. On a series of zirconium-based MOFs as model systems, we demonstrated the ability to capture and retain >99% of the transuranic Am radionuclide after 1 week of storage. We report the possibility of tailoring radionuclide release kinetics in MOFs through framework defects as a function of postsynthetically installed organic ligands including cation-chelating crown ether-based linkers.

Improved field-portable system to measure Cs-137 in wildlife.

We have developed an improved system to measure Cs-137 in wildlife at the Savannah River Site. This field-portable system consists of a shielded 5 cm by 10 cm by 40 cm NaI detector controlled by an Ametek Ortec Digibase. Measurement of an animal's radioactivity is made by placing the animal at a predefined location on the detector system for a one minute count-time.

Targeting complex plutonium oxides by combining crystal chemical reasoning with density-functional theory calculations: the quaternary plutonium oxide CsPuSiO.

The stability of the novel Pu(iv) silicate, Cs2PuSi6O15, was predicted from a combination of crystal chemical reasoning and DFT calculations and confirmed by its synthesis via flux crystal growth. Formation enthalpies of the A2MSi6O15 (A = Na-Cs; M = Ce, Th, U-Pu) compositional family were calculated and indicated the Cs-containing phases should preferentially form in the Cmc21 structure type, consistent with previous experimental findings and the novel phases produced in this work, Cs2PuSi6O15 and Cs2CeSi6O15. The formation enthalpies of a second set of compositions, A2MSi3O9, were also calculated and a comparison between the two compositional families correctly predicted A2MSi6O15 to be on average more stable than A2MSi3O9.

Expansion of the Na M (Ln/An) F Series: Incorporation of Plutonium into a Highly Robust and Stable Framework.

Na MAn F is an extremely versatile framework structure for incorporating tetravalent actinides (An) and cerium along with divalent or trivalent d-metals (M); moreover, the structure exhibits a high resistance to harsh chemical conditions. This extreme robustness can potentially be exploited for the sequestration of plutonium in a stable matrix; however, no Na MPu F compounds have been reported so far. Herein, we present four new plutonium fluorides that have been prepared as single crystals by mild hydrothermal synthesis methods.

"Boarding-Up": Radiation Damage and Radionuclide Leaching Kinetics in Linker-Capped Metal-Organic Frameworks.

For the first time, we report the ability to control radionuclide species release kinetics in metal-organic frameworks (MOFs) as a function of postsynthetic capping linker installation, which is essential for understanding MOF potential as viable radionuclide wasteform materials or versatile platforms for sensing, leaching, and radionuclide sequestration. The radiation damage of prepared frameworks under γ radiation has also been studied. We envision that the presented studies are the first steps toward utilization of the reported scaffolds for more efficient nuclear waste administration.

Long-term radiostrontium interactions and transport through sediment.

Radioactive strontium is one of the most common radiological contaminants in groundwater and soil. Objectives of this study were to (1) evaluate Sr transport through an 11-year-long field lysimeter study and (2) quantify secondary aging effects between Sr and sediment that may need to be considered for long-term transport modeling. Batch sorption/desorption tests were conducted with (85)Sr, (88)Sr, and (90)Sr using a sediment recovered from a field lysimeter containing a glass pellet amended with high-level nuclear waste for 24 years.

Aqueous (99)Tc, (129)I and (137)Cs removal from contaminated groundwater and sediments using highly effective low-cost sorbents.

Technetium-99 ((99)Tc), iodine-129 ((129)I), and cesium-137 ((137)Cs) are among the key risk-drivers for environmental cleanup. Immobilizing these radionuclides, especially TcO4(-) and I(-), has been challenging. TcO4(-) and I(-) bind very weakly to most sediments, such that distribution coefficients (Kd values; radionuclide concentration ratio of solids to liquids) are typically <2 mL/g; while Cs sorbs somewhat more strongly (Kd ∼ 50 mL/g).

Evaluation of a radioiodine plume increasing in concentration at the Savannah River Site.

Field and laboratory studies were carried out to understand the cause for steady increases in (129)I concentrations emanating from radiological basins located on the Savannah River Site, South Carolina. The basins were closed in 1988 by adding limestone and slag and then capping with a low permeability engineered cover. Groundwater (129)I concentrations in a well near the basins in 1993 were 200 pCi L(-1) and are presently between 400 and 1000 pCi L(-1).

Effect of quench on alpha/beta pulse shape discrimination of liquid scintillation cocktails.

The objectives of this paper are (1) to illustrate that knowledge of the external quench parameter is insufficient to properly setup a pulse shape discriminating liquid scintillation counter (LSC) for quantitative measurement, (2) to illustrate dependence on pulse shape discrimination on the radionuclide (more than just radiation and energy), and (3) to compare the pulse shape discrimination (PSD) of two commercial instruments. The effects various quenching agents, liquid scintillation cocktails, radionuclides, and LSCs have on alpha/beta pulse shape discriminating liquid scintillation counting were quantified. Alpha emitting radionuclides (239)Pu and (241)Am and beta emitter (90)Sr/(90)Y were investigated to quantify the nuclide dependence on alpha/beta pulse shape discrimination.

Influence of pH on plutonium desorption/solubilization from sediment.

Aqueous Pu concentrations and oxidation state transformations as a function of pH were quantified and compared between sorption/desorption studies and literature solubility values. When Pu(V) was added to a red subsurface sandy-clay-loam sediment collected near Aiken, South Carolina, 99% of the Pu sorbed to the sediment within 48 h. Throughout the study, > or = 94% of the Puaq remained as Pu(V), whereas < or = 6% was Pu(VI) and < or = 1% was Pu(IV).

Compression ultrasonography. Treatment for acute femoral artery pseudoaneurysms in selected cases.

Treatment of pseudoaneurysms has traditionally been surgical. We evaluated 12 patients who developed femoral artery pseudoaneurysms after cardiac catheterization. Using color Doppler ultrasonography steady pressure was applied, occluding flow in both the neck and body of the pseudoaneurysm for 10 minute intervals.

Acute renal insufficiency due to renal infarctions in a patient with neurofibromatosis.

Manifestations of neurofibromatosis in the skin, the eye, and the skeletal and nervous systems have been well documented since the disease was first described in 1882. Stenosing vascular lesions as complications of neurofibromatosis were first reported in 1945. They are being increasingly recognized and most commonly involve the renal artery.