Batch data for the sorption of Eu and Th on pelagic sediments may be represented by equations of the form: ln M = A ln Cs + B/T + D, where M = concentration of sorbate on sediment, Cs = concentration of sorbate in solution, T = absolute temperature, and A, B, and D = constants. Thermodynamic interpretation of this equation leads to an expression for the true thermodynamic equilibrium constant of K = m/CsA and for the enthalpy change, ΔH, of d ln(M/CsA)/d(1/T) = −ΔH/R, where R = universal gas constant.

Experimentally, the sorption of Eu onto clay-rich sediments was very rapid in the first few seconds and slowed over an interval of minutes to hours. Rate curves were similar in shape to those of α-iron hydroxide, rather than of the oxalate-extracted residual sediment, indicating the importance of oxyhydroxide-like phases in the uptake of Eu onto red-clay sediments. For clay-rich sediments, numerical modeling reproduced the general features of a series of diffusion experiments. To a first approximation, the penetration of Eu into a sediment proceeded by saturation of the sediment to the depth of penetration and produced a sharp drop-off in sorbed + dissolved Eu concentration at the diffusion front. Higher partition coefficients (Kp) resulted in greater sorbed + dissolved concentrations, but reduced penetration. For calcareous sediments, however, Eu concentrations at the surface were much higher than at depth, presumably due to the formation of an insoluble carbonate.

The alteration and transformation behaviour of Ceca smectite in two acid and saline solutions (NaCl and KCl) was studied in batch experiments. This type of smectite is proposed as potential backfill material for nuclear waste storage sites. The initial solution was enriched with 500 ppm of U, Th and Eu. The evolution of pH and solution concentrations were measured over a period of 25 months. The mineralogical and chemical evolution of the clays was also studied. X-ray diffraction revealed a significant loss of diffraction intensity and the clays became amorphous to Xrays with increasing reaction time. Deconvolution of the XRD data indicated a continuous collapse of the smectite layers but no illitization. Infrared spectroscopy revealed unchanged smectite spectra at the end of the experiment. Thorium precipitated as amorphous ThO2, but showed an incipient crystallization after 500 days. The Th, Eu and U were neither adsorbed onto the clays nor incorporated into a secondary phase.

Monazite is a light rare-earth element (LREE)-bearing accessory phase common in felsic granitic rocks, and strongly influences LREE concentrations in granites and the chemistry of melts and residues formed during partial melting. Cheralite-rich (high-Th) monazite-(Ce) has been recorded as rims on partially dissolved cores in a suite of granulite-facies migmatites generated by disequilibrium melting. High-Th monazite has previously been recorded only in granitic-pegmatite occurrences. Subidiomorphic monazite-(Ce) from leucosome, melanosome and mesosome consists of complexly zoned cores (up to 300 µm in diameter) containing 5.17–9.87 wt.% ThO2, overgrown by essentially unzoned rims (containing up to 21.4 wt.% ThO2). Uranium contents are average for Th-rich monazite-(Ce) (0.22–3.17 wt.% UO2). Th enrichment (relative to LREE) in monazite-(Ce) rims is ascribed to the presence of fluorine-bearing melts (formed during the incongruent breakdown of biotite to produce a water-undersaturated melt), allowing the formation of REE-fluoride complexes in the melt, coupled with the increased charge balanced substitutions Th4+ + Si4+ ⇌ REE3+ + P5+ and Th4+ + Ca2+ ⇌ 2REE3+ into monazite-(Ce). Fractionation of Th and U (reflected by an increased in Th/U in rims relative to cores) may have occurred due to the removal by a CO2-rich fluid phase in the melt. These interpretations are consistent with elevated CO2 and F contents of granitic liquids produced during the water-undersaturated breakdown of biotite under granulite-facies conditions. Evidence for restricted monazite-(Ce)-melt equilibration and rapid melt removal is provided by the ubiquitous presence of partially embayed cores and unzoned rims.

The effect of competition from other metal ions on the complexation of Ni with isosaccharinic acid, gluconic acid and picolinic acid, at high pH, is described. The competing metal ions used were divalent Co, trivalent Eu and tetravalent Th. In the majority of cases, competition from these metal ions followed the predicted pattern, with most anomalies seeming to be caused by sorption of Ni to the many different solid phases formed in presence of the competing ions. The Ni solid phase was shown to change with time during the course of the study. No major unexplained competition effects were found.

The sorption behaviour of I−, Cs+, Ni2+, Eu3+, Th4+ and UO2+ 2on NRVB (Nirex reference vault backfill) a possible vault backfill, at pH 12.8 was studied. Sorption isotherms generated were compared to results obtained in the presence of cellulose degradation products (CDP). Whereas Cs was not affected by the presence of the organic compounds, a notable reduction in the sorption of Th and Eu to cement was observed. The results also indicated limited removal of Ni from solution (with or without an organic ligand) by sorption, the concentration in solution seemingly being determined solely by solubility processes. In the case of uranium, the presence of CDP increased the sorption to cement by almost one order of magnitude. Further studies into the uptake of CDP by cement are being undertaken to identify the mechanism(s) responsible.

The Llandovery Folly Sandstone near Presteigne, Powys, contains disseminated thorium mineralization. The thorium occurs as inclusions of thorite and thorianite within sub-millimetre-scale bitumen nodules throughout the sandstone. The nodules grew replacively in situ. The two square kilometres outcrop/subcrop of the sandstone may contain over 500 tonnes thorium.

Th- and Zr-bearing perovskite and Zr-rich Ti garnet are described from the Polino calcite carbonatite, Italy. The garnets contain 6.05-7.50 wt.% ZrO2 in cores and up to 15.80 wt.% in rims. Silicon is low in these garnets and substantial Al and Fe 3+ has been assigned to the tetrahedral sites. A strong correlation of Si with Zr from published data suggests the possibility that some Zr may also be tetrahedrally coordinated. However, the chemistry alone does not constrain the site distribution of Fe, Ti, Zr and Mg unambiguously. The perovskites are very unusual in containing 2.81-3.27 wt.% ZrO2 and 1.48-1.71 wt.% ThO2. For comparison, new analyses are presented of the zirconium garnet kimzeyite and coexisting perovskite from the type locality at Magnet Cove.

Six hundred and forty four gamma-ray spectrometer assays of U and Th obtained within the late Caledonian Galway Granite western Ireland are presented. The data cover the range of granodiorites, adamellites and leucogranites (Murvey Granite) present in the batholith. There is an overall increase in U and Th abundances with petrological evolution. The broad scatter of values that characterizes the Murvey Granite reflects the geographically separate occurrences of this leucogranite. Rubidium and strontium data imply varying degrees of fractionation among these separate Murvey Granite occurrences. Y and HREE are notably enriched in the Murvey granite at Costelloe which also contains the highest Th levels amongst the leucogranites. Thorite, uraninite, monazite and Y-zircon are present in this leucogranite and are responsible for the observed enrichments in U, Th, Y and HREE.

Cellulose degradation products (CDPs) can complex with radioelements causing solubility enhancement and sorption reduction, effects which are detrimental to the containment of radionuclides in the near field of a geological disposal facility and surrounding geosphere. Isosaccharinic acid (ISA) is the principal component of CDPs formed under the alkaline anaerobic conditions of a cement-based near field and appears to be largely responsible for the impact of CDPs on radionuclide solubility and sorption under near-field conditions. However, the situation appears to be more complicated under near-neutral pH geosphere conditions.

A combined experimental and modelling study was undertaken to compare the impact of a CDP leachate to ISA in a simple model ternary sorption system consisting of hematite as a single mineral substrate, thorium as the radioelement and ISA or a CDP leachate as the complexant. Thorium sorbs strongly to hematite. A triple layer model for thorium sorption to hematite was refined to fit to the experimental data in the absence of ISA or CDP leachate; the effect of ISA on thorium sorption was then predicted.

In the presence of CDP leachate, a significant reduction in thorium sorption was observed from pH 6 to 12 in good agreement with model predictions based on a high concentration of ISA. However, only a limited impact of ISA on thorium sorption was observed at pH 6 to 12, in contrast to predictions. The effects of ISA could be accounted for by assuming the formation of a ternary thorium–ISA–surface complex. The model has yet to be extended to the more complex CDP systems. Differences in the thorium speciation in solution due to the formation of a ternary calcium–thorium–ISA complex in the CDP leachate, which is absent from solutions with ISA only, provides the most likely explanation for the differences observed experimentally.

Materials designed for nuclear waste disposal include a range of ceramics, glass ceramics and glass waste forms. Those with crystalline phases have provided the momentum for studies of minerals as a means to understand aspects of waste-form crystal chemistry, behaviour in aqueous systems and radiation damage over geological periods of time. Although the utility of natural analogue studies varies, depending upon the degree of analogy to the proposed geological repository and other factors such as chemical composition, the available data suggest that Th-U host phases such as brannerite, monazite, pyrochlore, zircon and zirconolite are resistant generally to dissolution in aqueous fluids at low temperatures. Geochemical durability may or may not extend to hydrothermal systems depending on the specifics of fluid composition, temperature and pressure. At elevated temperatures, for example, davidite may break down to new phase assemblages including titanite, ilmenite and rutile. Perovskite is generally less resistant to dissolution at low temperatures and breaks down to TiO2, releasing A-site cations to the aqueous fluid. Studies of radiation damage indicate that the oxide and silicate phases become amorphous as a result of the gradual accumulation of alpha-recoil collision cascades. Monazite tends to remain crystalline on geological time scales, a very attractive property that potentially eliminates major changes in physical properties such as density and volume, thereby reducing the potential for cracking, which is a major concern for zircon. In spite of recent success in describing the behaviour of Th-U minerals in geological systems, considerable work remains in order to understand the P-T-X conditions during alteration and T-t history of the host rocks.

A Th-rich mineral of the crandallite group has been investigated from the weathering profile of the Schugorsk bauxite deposit, Timan, Russia. It occurs within thin (up to 0.5 mm) organic-rich veinlets together with ‘leucoxene’ in the form of small shapeless grains which vary in size from 1—2 mm to 60—70 mm. Rare grains disseminated among boehmite crystals were also found. Microprobe analyses determined that the ThO2 content can be as high as 18 wt.%. The mineral composition is intermediate between crandallite CaAl3H(PO4)2(OH)6, goyazite SrAl3H(PO4)2(OH)6, Th-crandallite and svanbergite SrAl3PO4SO4(OH)6 in the beudantite group.

Comparatively high contents of Fe and Si and a very high positive Th and Fe content correlation (r = +0.98) suggest that the formula of the hypothetical Th-bearing end-member is ThFe3(PO4,SiO4)2(OH)6 with Th and Si substituting for REE and Prespectively (woodhouseite-type substitution). Another possible substitution is Th4+ + Ca2+ ⇋ 2REE3+ (florencite-type). A deficiency of cations in the X site can be explained by either the presence of carbon, undetectable by microprobe, in the crystal lattice or a lack of X-site cations due to radiation damage induced by Th. Some excess of cations in the B site (Al and Fe3+) can be explained by the presence of very small boehmite and hematite inclusions on the crandallite grain surfaces. Th-rich crandallite may be the result of alteration of an unidentified silicate mineral from the parent rock with a composition close to the simplified formula Fe2+ThSiO4(OH)2.

The Fen Complex in Norway consists of a ~583 Ma composite carbonatite-ijolite-pyroxenite diatreme intrusion. Locally, high grades (up to 1.6 wt.% total REE) of rare-earth elements (REE) are found in a hydrothermally altered, hematite-rich carbonatite known as rødbergite. The progressive transformation of primary igneous carbonatite to rødbergite was studied here using scanning electron microscopy and inductively coupled plasma-mass spectrometry trace-element analysis of 23 bulk samples taken along a key geological transect. A primary mineral assemblage of calcite, dolomite, apatite, pyrite, magnetite and columbite with accessory quartz, baryte, pyrochlore, fluorite and REE fluorocarbonates was found to have transformed progressively into a secondary assemblage of dolomite, Fe-dolomite, baryte, Ba-bearing phlogopite, hematite with accessory apatite, calcite, monazite-(Ce) and quartz. Textural evidence is presented for REE fluorocarbonates and apatite breaking down in igneous carbonatite, and monazite-(Ce) precipitating in rødbergite. The importance of micro-veins, interpreted as feeder fractures, containing secondary monazite and allanite, is highlighted. Textural evidence for included relics of primary apatite-rich carbonatite are also presented. These acted as a trap for monazite-(Ce) precipitation, a mechanism predicted by physical-chemical experiments. The transformation of carbonatite to rødbergite is accompanied by a 10-fold increase in REE concentrations. The highest light REE (LREE) concentrations are found in transitional vein-rich rødbergite, whereas the highest heavy REE (HREE) and Th concentrations are found within the rødbergites, suggesting partial decoupling of LREE and HREE due to the lower stability of HREE complexes in the aqueous hydrothermal fluid. The hydrothermal fluid involved in the formation of rødbergite was oxidizing and had probably interacted with country-rock gneisses. An ore deposit model for the REE-rich rødbergites is presented here which will better inform exploration strategies in the complex, and has implications for carbonatite-hosted REE resources around the world.

The chronology of Quaternary paleoenvironment and climate in northeastern Siberia is poorly understood due to a lack of reliable numerical age determinations. The best climatic archives are ice-rich permafrost sequences, which are widely distributed in northeastern Siberia. For this study, 230Th/U-ages were determined by thermal ionization mass spectrometry (TIMS) from frozen peat in a permafrost deposit at the southern cliff of the Bol'shoy Lyakhovsky Island (New Siberian Archipelago), west of the Zimov'e River. These yielded a Pre-Eemian “isochron”-corrected 230Th/U-age of 200,900±3400 yr. This result is reliable because permafrost deposits behave as closed systems with respect to uranium and thorium. Our findings suggest that 230Th/U dating of frozen peat in permafrost deposits is a useful tool for the reconstruction of the Middle Quaternary environment of northern Siberia and of the whole Arctic.

The insertion of reprocessed fuel spiked with thorium in a typical PWR fuel element considering (TRU-Th) cycle was simulated using different fissile materials that varied from 5.5% to 7.0%. The reprocessed fuels were obtained using the ORIGEN 2.1 code from a burned PWR standard fuel (33,000 MWd/tHM burned), with 3.1% of initial enrichment, which was remained in the cooling pool for five years and then reprocessed using UREX+ technique. The kinf, hardening spectrum and the fuel evolution during the burnup were evaluated. This study was performed using the SCALE 6.0

In France, the activities carried out by the “small-scaleholders” of nuclear materials are organized by a specific regulatorysystem which defines in a detailed way their obligations and themeans of control of the government. The first part of the articlepresents the legal framework relating to the use of nuclear materialsby small-scale holders in civilian fields. The importance of thedeclaration of the nuclear material inventory is clearly emphasizedand must be prepared and transmitted to the Institute for RadiologicalProtection and Nuclear Safety (IRSN) every year. The second partdescribes how this declaration is used to provide basic informationfor the competent Ministry and the inspectors to check the correct applicationof the regulatory requirements relating to physical protection andto the control of nuclear materials. Finally, the last part presentsthe on-site inspections carried out by sworn and accredited inspectorsunder the authority of the competent Authority, which provide anoverall picture and allow an evaluation of the risks of theft, lossor diversion of these materials.

An epidemiology study on lung cancer mortality of the dust-exposed miners and dust-unexposed miners (controls) was performed in 2001. It was found that, during the period from 1977 to March 2001, 27 cases of lung cancers were observed in the dust-exposed miners, while 8 cases of lung cancers were found in controls. The SMRs of them were 6.13 and 1.90 respectively. The SMR of the dust-exposed miners was much higher than that of the controls. The difference between the two SMRs is very significant (χ2 = 9.488, P < 0.005). The probability that 27 or more lung cancers would occur in the dust-exposed group, given the expected numbers and that a total of 35 occurred is 0.0015. The high SMR for lung cancers among dust-exposed miners likely resulted from the inhaled thorium-containing dusts (carcinogens are ThO2 and SiO2) and its short lived thoron progeny. This is the first evidence in humans of the carcinogenicity after long-term inhalation of thorium-containing dusts and thoron progeny. The total person-years of observation of the dust exposed miners and the unexposed miners were 62 712 and 34 672 respectively.

Uranium (238U) and thorium (232Th) concentrations were measured in different foods widely consumed in Morocco by using CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs). Data obtained were compared to those obtained by using isotope dilution mass spectrometry (IDMS). Total daily intakes of 238U and 232Th for a typical food basket were estimated to be 1.3 ± 0.1 mBq d-1 and 0.98 ± 0.08 mBq d-1, 1.4 ± 0.1 mBq d-1 and 1.06 ± 0.08 mBq d–1, 1.7 ± 0.1 mBq d–1 and 1.26 ± 0.08 mBq d–1 and 2.0 ± 0.1 mBq d–1 and 1.5 ± 0.1 Bq d–1 for the 2–7 years, 7–12 years, 12–17 years and adult’s age groups, respectively. Alpha-activities due to annual 238U and 232Th intakes from the ingestion of the studied foodstuffs were determined in different organs and tissues of the human body of members of the public by using the ICRP gastrointestinal tract and systemic part models for these radionuclides. Committed equivalent doses due to annual intakes of 238U and 232Th were evaluated in the human body organs and tissues for different age groups of the Moroccan population by exploiting data obtained for alpha-doses deposited by 1 Bq of 238U and 1 Bq of 232Th in the considered human organs and tissues. The influence of the mass of the target tissue and activities due to 238U and 232Th on the committed equivalent doses due to annual intakes of these radionuclides in the organs and tissues of the human body was studied.

En 2000, des flux de rayonnement anormalement élevés ont été détectés sur certaines plages du littoral camarguais. Les sables du littoral camarguais ont alors fait l’objet d’une caractérisation radiologique montrant des activités moyennes de quelques dizaines de Bq kg-1 en uranium-238 et thorium-232 d’une part, et l’existence de points chauds à plus de 1000 Bq kg-1 d’autre part ; voire plus sur deux plages : l’une située à l’Est du phare de Beauduc, l’autre située à l’Est du phare de l’Espiguette. Cette radioactivité, d’origine naturelle, est responsable de l’exposition des personnes fréquentant ces deux dernières plages relativement isolées, mais néanmoins accessibles à tout public. L’Institut de radioprotection et de sûreté nucléaire a réalisé une évaluation des doses susceptibles d’être reçues par des personnes fréquentant ces deux dernières plages, en se basant sur des mesures et des prélèvements effectués in situ, en établissant expérimentalement la solubilité des sables dans les fluides gastrique et intestinal, et en formulant des hypothèses sur la fréquentation des lieux (scénarios). La dose annuelle maximale ainsi évaluée est de l’ordre de 0,8 mSv pour des adultes et 0,5 mSv pour les enfants ; valeurs vraisemblablement très prudentes dans lesquelles la dose par exposition externe prédomine largement.

A twenty-year follow-up study was carried out at Baiyun Obo Rare-earth Iron Mine in China, This mine has been mined since 1958. Its ore contains 0.04% of ThO2 and 10% of SiO2. The purpose of this study is to investigate possible health effects in dust-exposed miners following long-term exposure to thorium-containing dusts and thoron progeny. By using the negative high voltage exhaled thoron progeny measurement system to estimate the miner’s thorium lung burden. The highest thorium lung burden among 1 158 measurements of 638 miners was 11.11 Bq. The incidence of stage 0+ pneumoconiosis was increased among dust-exposed miners. An epidemiological study showed that the lung cancer mortality of the dust-exposed miners was significantly (p < 0.005) higher than that of the non-exposed group. It is suggested that the difference results in the long-term exposure to thorium-containing dusts (carcinogens are ThO2 and SiO2) and thoron progeny. This is the first evidence in humans of the carcinogenicity after long-term inhalation of thorium-containing dusts and thoron progeny. The total person-years of observation for the dust-exposed miners and the controls were 62 712 and 34 672 respectively.