A comparative bio-oxidative leaching study of synthetic U-bearing minerals: Implications for mobility and retention.

In this study, the effects of bio-oxidative leaching on several synthetic uranium minerals - Uraninite [UO2], Pitchblende [U3O8], Coffinite [USiO4], Brannerite [UTi2O6] and Betafite [(U,Ca)2(Ti,Nb,Ta)2O7]) compared to chemical leaching in the presence of pyrite was investigated. In all cases, bio-oxidative leaching was faster and increased overall %U extraction compared to chemical leaching. The results indicated that the bio-oxidative leachability of the uranium minerals was in the order: pitchblende≈ uraninite > coffinite>> brannerite > betafite. The leaching of pitchblende and uraninite was fast and complete; U extraction from coffinite was slower over 28 days' during the bioleaching. The use of thermophiles doubled the recovery of U from refractory brannerite. The results highlight the significant capability of bio-leaching in the recovery of U from brannerite; both mesophilic and thermophilic bacteria was found to enhance U recovery likely through enhanced breakdown of the titanate structure. Brannerite is often found in significant quantities within ore tailings due to its refractory nature, which can lead to subsequent release of U into the environment. Conversely, betafite is highly stable in the presence of mesophile and moderate thermophiles, which suggested that betafite materials can be a viable future host for long term storage for spent nuclear fuels.

Modelling the dispersion of radionuclides in dust from a landform covered by low uranium grade waste rock.

The dispersion of radionuclides in dust and inhalation dose rates to the public from the planned remediation of the Ranger uranium mine in the wet-dry tropics of Australia was modelled using RESRAD-OFFSITE. Dust inhalation dose rates were predicted to be highest on the remediated site and decrease with an approximate inverse square to inverse cubic dependence with distance from the site. The annual dose above natural background to a hypothetical individual permanently occupying the remediated site (representing the worst case scenario for radionuclide in dust exposure) was estimated to be 5.3 × 10-3 mSv. The estimated doses from exposure to radionuclides in dust were two to three orders of magnitude lower than those from exposure to 222Rn. A sensitivity analysis showed that source-related and receptor-related model parameters had direct proportional influences on dust inhalation dose rates. Four transport-related model parameters (atmospheric stability class, deposition velocity of particulates, precipitation and wind speed) were also influential and generally had an increasing influence with distance from the source. The results of this study may provide general guidance to similar sites elsewhere on the relative importance of dust versus gaseous 222Rn transport pathways and the relative influence of dispersion modelling parameters on predicted exposures and doses.

Modelling the dispersion of radon-222 from a landform covered by low uranium grade waste rock.

The dispersion of 222Rn from the planned remediation of the Ranger U mine in the wet-dry tropics of Northern Australia was modelled. Dry and wet season contour maps of 222Rn dose normalised to 226Ra activity concentration in the proposed waste rock substrate on the remediated landform were developed. Three example exposure scenarios were assessed based on an anticipated waste rock 226Ra activity concentration of 800 Bq kg-1. The estimated above-background annual dose from 222Rn to hypothetical receptors at the Aboriginal community at Mudginberri (∼10 km NNW) was 0.005 mSv and at the township of Jabiru (∼7 km W) was 0.033 mSv. The estimated above-background annual dose for the hypothetical worst case scenario, representing a receptor 1 km WNW of the landform centroid during the dry season and at the centroid during the wet season, was 0.13 mSv. Variability analysis on the 20 y meteorological dataset used in the dispersion modelling showed that the dry and wet season 222Rn dose predictions in any single year could be approximately double those of an average year, which suggests that estimates of average 222Rn dose should potentially be doubled if the assessment aim is to demonstrate compliance with the public dose limit.

Radionuclide disposal using the pyrochlore supergroup of minerals as a host matrix-A review.

Since the first large scale commercial nuclear power plant became operational in 1958, the nuclear power industry has been faced with the growing problem of disposal of radionuclides produced from nuclear fission. The current global production of high level nuclear waste is approximately 10,000 metric tons p.a., consisting predominantly of uranium, plutonium, actinides and other minor radionuclides. Developing a safe and cost-effective method for long term storage and disposal of nuclear waste is a key issue of concern to the nuclear power industry. A promising approach to radionuclide disposal is incorporation of the nuclear waste into refractory oxide host minerals or mineral matrices. This technique offers lower leaching rates when compared to the commonly used glass-based vitrification approaches. The refractory pyrochlore supergroup of minerals are particularly attractive for this purpose as they can incorporate considerable amounts of the radionuclides: 93Zr, 133Ba, 135Cs, Th, U, 238Pu, and 244Cm, while demonstrating very low leachability. This review examines the structural, compositional and chemical properties of radionuclide-containing pyrochlore supergroup minerals. Compiled leaching data for radionuclides hosted in pyrochlores demonstrates that these materials offer a high degree of aqueous durability making them strong candidates for radionuclide disposal, offering a viable storage alternative to traditional vitrification methods.

Synthesis and characterisation of the uranium pyrochlore betafite [(Ca,U)2(Ti,Nb,Ta)2O7].

Betafite of composition [(Ca,U)2(Ti,Nb,Ta)2O7] was prepared via a solid state synthesis route. The synthesis was shown to be sensitive to initial reactant ratios, the atmosphere used (oxidising, neutral, reducing) and time. The optimum conditions for the synthesis of betafite were found to be heating the reactants required at 1150°C for 48 h under an inert gas atmosphere. XRD characterisation revealed that the synthesised betafite contained minor impurities. EPMA analysis of a sectioned surface showed very small regions of Ca-free betafite on grain boundaries as well as minor rutile impurities. Some heterogeneity between the Nb:Ta ratio was observed by quantitative EPMA but was generally within the nomenclature requirements stated for betafite. SEM analysis revealed the synthesised betafite was comprised mostly of hexaoctohedral crystals of ∼ 3 µm in diameter. XPS analysis of the sample showed that the uranium in the synthesised betafite was predominately present in the U(5+) oxidation state. A minor amount of U(6+) was also detected which was possibly due to surface oxidation.