Apatite- and Monazite-Bearing Glass-Crystal Composites for the Immobilization of Low-Level Nuclear and Hazardous Wastes

This study demonstrates that glass-crystal composite waste forms can be produced from waste streams containing high proportions of phosphorus, transition metals, and/or halides. The crystalline phases produced in crucible-scale melts include apatite, monazite, spinels, and a Zr-Si-Fe-Ti phase. These phases readily incorporated radionuclide and toxic metals into their crystal structures, while corrosion tests have demonstrated that glass-crystal composites can be up to 300-fold more durable than simulated high-level nuclear waste glasses, such as SRL 202U

Sophomore and Junior Recital: Viola Trio

Kemp Recital HallApril 19, 2014Saturday Evening7:30 p.m

Alpha and gamma radiation effects on air-water systems at high gas/liquid ratios

Radiolysis tests were conducted on air-water systems to examine the effects of radiation on liquid phase chemistry under high gas/liquid volume (G/L) ratios that are characteristic of an unsaturated nuclear waste repository setting. Test parameters included temperatures of 25, 90, and 200{degrees}C; gamma vs. alpha radiation; dose rates of {approximately}3500 and 50,000 rad/h; and G/L ratios of 10 and 100. Formate, oxalate, and total organic carbon contents increased during irradiation of the air-water systems in gamma and alpha tests at low-dose rate ({approximately}3500 rad/h). Increases in organic components were not observed for tests run at 200{degrees}C or high-dose rates (50,000 rad/h). In the tests where increases in organics occurred, the formate and oxalate were preferentially enriched in solutions that were rinsed from the test vessel walls. Nitrate (NO{sub 3}{sup {minus}}) is the dominant anion produced during the radiolysis reactions. Significant nitrite (NO{sub 2}{sup {minus}}) also occurs in some high-dose rate tests, with the reduced form of nitrogen possibly resulting from reactions with the test vessels. These results indicate that nitrogen acids are being produced and concentrated in the limited quantities of solution present in the tests. Nitrate + nitrite production varied inversely with temperature, with the lowest quantities being detected for the higher temperature tests. The G(NO{sub 3}{sup {minus}} + NO{sub 2}{sup {minus}}) values for the 25, 90, and 200{degrees}C experiments with gamma radiation are 3.2 {+-} 0.7, 1.3 {+-} 1.0, and 0.4 {+-} 0.3, respectively. Thus, the elevated temperatures expected early in the life of a repository may counteract pH decreases resulting from nitrogen acid production. Little variation was observed in G values as a function of dose rate or gas/liquid ratio

Grain boundary corrosion and alteration phase formation during the oxidative dissolution of UO{sub 2} pellets

Alteration behavior of UO{sub 2} pellets following reaction under unsaturated drip-test conditions at 90 C for up to 10 years was examined by solid phase and leachate analyses. Sample reactions were characterized by preferential dissolution of grain boundaries between the original press-sintered UO{sub 2} granules comprising the samples, development of a polygonal network of open channels along the intergrain boundaries, and spallation of surface granules that had undergone severe grain boundary corrosion. The development of a dense mat of alteration phases after 2 years of reaction trapped loose granules, resulting in reduced rates of particulate U release. The paragenetic sequence of alteration phases that formed on the present samples was similar to that observed in surficial weathering zones of natural uraninite (UO{sub 2}) deposits, with alkali and alkaline earth uranyl silicates representing the long-term solubility-limiting phases for U in both systems

Apatite- and Monazite-Bearing Glass-Crystal Composites for the Immobilization of Low-level Nuclear and Hazardous Wastes

This study demonstrates that glass-crystal composite waste forms can be produced from waste streams containing high proportions of phosphorus, transition metals, and/or halides. The crystalline phases produced in crucible-scale melts include apatite, monazite, spinels, and a Zr-Si-Fe-Ti phase. These phases readily incorporated radionuclide and toxic metals into their crystal structures, while corrosion tests have demonstrated that glass-crystal composites can be up to 300-fold more durable than simulated high-level nuclear waste glasses, such as SRL 202U

Plutonium Silicate Alteration Phases Produced by Aqueous Corrosion of Borosilicate Glass

Borosilicate glasses loaded with {approx}10 wt % plutonium were found to produce plutonium-silicate alteration phases upon aqueous corrosion under a range of conditions. The phases observed were generally rich in lanthanide (Ln) elements and were related to the lanthanide orthosilicate phases of the monoclinic Ln{sub 2}SiO{sub 5} type. The composition of the phases was variable regarding [Ln]/[Pu] ratio, depending upon type of corrosion test and on the location within the alteration layer. The formation of these phases likely has implications for the incorporation of plutonium into silicate alteration phases during corrosion of titanate ceramics, high-level waste glasses, and spent nuclear fuel

Constraints on the Geological History of the Karst System in Southern Missouri, U.S.A. Provided by Radiogenic, Cosmogenic and Physical/Chemical Characteristics of Doline Fill

Območje Ozarkov v južnem Missouriju gradijo predvsem karbonatne, morske, platformne kamnine paleozojske starosti. Teren, ki vsebuje obširen kras, predstavlja kopno že od poznega Paleozojka. Da bi bolje razumeli geološko zgodovino tega kraškega sistema, smo raziskali stratigrafske podatke ohranjene v zapolnitvi velike vrtače pri največjem izviru v okolici. Vzorci zapolnitve iz naravnih izdankov in iz vrtine so bili analizirani s termoluminiscenco (TL) in 10Be kozmogeno metodo. Fizikalno-kemijske značilnosti zapolnitve so bile določene vizualno, z rentgensko metodo in merjenjem velikosti delcev. Podatki vrtine kažejo, da je debelina alohtonega materiala, ki zapolnjuje vrtačo 36,3 m. Ta material prekriva podorne bloke in sedimente debeline vsaj 15,6 m. Glede na teksturo, strukturo in barvo delimo material, ki zapolnjuje vrtačo na 7 con. Analize 10Be koncentracij kažejo, da material za celotni stolpec zapolnitve izvira iz rezidualnega materiala iz srednjega (Illinoian) in zgornjega Pleistocena (Wisconsian). Rentgenske analize glin kažejo, da zapolnitev vrtače vsebuje enake količine kaolinita in illita, kar je skladno z zemeljskim preperevanjem.The Ozark Plateaus region of southern Missouri is underlain by dominantly carbonate marine platform rocks of Paleozoic age. The region has been sub-aerially exposed since the late Paleozoic and is characterized by extensive karst. To better understand the geologic history of this regional karst system, we examined the stratigraphic record preserved in the fill of a large doline near the largest spring in the region. Samples of fill from natural exposures and drill core were analyzed using thermoluminescence (TL) and 10Be cosmogenic techniques, and the physical/chemical characteristics of the fill material were determined by visual inspection, X-ray analyses, and grain-size measurements. Drill-hole data indicate that the allochthonous doline fill is 36.3 m thick and rests on at least 15.6 m of cave breakdown and sediment. The doline fill is divisible into 7 zones. Analysis of 10Be concentrations suggest that the entire doline fill was derived from local residuum during the middle (Illinoian) to late Pleistocene (Wisconsinan). X-ray diffraction analyses of clays throughout the doline fill indicate that they consist of nearly equal amounts of kaolinite and illite, consistent with terrestrial weathering.

An Evaluation of Glass-Crystal Composites For the Disposal of Nuclear and Hazardous Waste Materials

Waste forms made of a glass-crystal composite (GCC) are being evaluated at Argonne National Laboratory for their potential use in the disposal of low-level nuclear and hazardous waste materials. This waste form is being developed within the framework strategy of DOE`s minimum Additive Waste Stabilization (MAWS) Program. The MAWS protocol involves the blending of multiple waste streams to achieve an optimal feed composition, which eliminates the need to use large amounts of additives to produce an acceptable waste form. The GCCs have a particularly useful utility in their ability to incorporate waste streams with high metal contents, including those that contain large amounts of scrap metals, and in their potential for sequestering radionuclide and hazardous constituents in corrosion-resistant mineral phases. This paper reports the results from tests conducted with simulated feeds representative of potential DOE and industry waste streams. Topics addressed include the partitioning of various radioactive and hazardous constituents between the glass and crystalline portions of the waste form, the development of secondary phases on the altered sample surfaces during corrosion testing, and the fate of waste components during corrosion testing, as indicated by elements released to solution and microanalysis of the reacted solid samples

Onboard Science Instrument Autonomy for the Detection of Microscopy Biosignatures on the Ocean Worlds Life Surveyor

The quest to find extraterrestrial life is a critical scientific endeavor with civilization-level implications. Icy moons in our solar system are promising targets for exploration because their liquid oceans make them potential habitats for microscopic life. However, the lack of a precise definition of life poses a fundamental challenge to formulating detection strategies. To increase the chances of unambiguous detection, a suite of complementary instruments must sample multiple independent biosignatures (e.g., composition, motility/behavior, and visible structure). Such an instrument suite could generate 10,000x more raw data than is possible to transmit from distant ocean worlds like Enceladus or Europa. To address this bandwidth limitation, Onboard Science Instrument Autonomy (OSIA) is an emerging discipline of flight systems capable of evaluating, summarizing, and prioritizing observational instrument data to maximize science return. We describe two OSIA implementations developed as part of the Ocean Worlds Life Surveyor (OWLS) prototype instrument suite at the Jet Propulsion Laboratory. The first identifies life-like motion in digital holographic microscopy videos, and the second identifies cellular structure and composition via innate and dye-induced fluorescence. Flight-like requirements and computational constraints were used to lower barriers to infusion, similar to those available on the Mars helicopter, "Ingenuity." We evaluated the OSIA's performance using simulated and laboratory data and conducted a live field test at the hypersaline Mono Lake planetary analog site. Our study demonstrates the potential of OSIA for enabling biosignature detection and provides insights and lessons learned for future mission concepts aimed at exploring the outer solar system.Comment: 49 pages, 18 figures, submitted to The Planetary Science Journal on 2023-04-2

Reproduction of natural corrosion by accelerated laboratory testing methods

Various laboratory corrosion tests have been developed to study the behavior of glass waste forms under conditions similar to those expected in an engineered repository. The data generated by laboratory experiments are useful for understanding corrosion mechanisms and for developing chemical models to predict the long-term behavior of glass. However, it is challenging to demonstrate that these test methods produce results that can be directly related to projecting the behavior of glass waste forms over time periods of thousands of years. One method to build confidence in the applicability of the test methods is to study the natural processes that have been taking place over very long periods in environments similar to those of the repository. In this paper, we discuss whether accelerated testing methods alter the fundamental mechanisms of glass corrosion by comparing the alteration patterns that occur in naturally altered glasses with those that occur in accelerated laboratory environments. This comparison is done by (1) describing the alteration of glasses reacted in nature over long periods of time and in accelerated laboratory environments and (2) establishing the reaction kinetics of naturally altered glass and laboratory reacted glass waste forms