ION FLOTATION OF INORGANIC IONS. 1. THE CONCENTRATION OF URANIUM.
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Ammonium Compounds↗
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Reduction of uranium(VI) by mixed iron(II)/iron(III) hydroxide (green rust): formation of UO2 nanoparticles.
Green rusts, which are mixed ferrous/ferric hydroxides, are found in many suboxic environments and are believed to play a central role in the biogeochemistry of Fe. Analysis by U LIII-edge X-ray absorption near edge spectroscopy of aqueous green rust suspensions spiked with uranyl (U(VI)) showed that U(VI) was readily reduced to U(IV) by green rust The extended X-ray absorption fine structure (EXAFS) date for uranium reduced by green rust indicate the formation of a UO2 phase. A theoretical model based on the crystal structure of UO2 was generated by using FEFF7 and fitted to the data for the UO2 standard and the uranium in the green rust samples. The model fits indicate that the number of nearest-neighbor uranium atoms decreases from 12 for the UO2 structure to 5.4 forthe uranium-green rust sample. With an assumed four near-neighbor uranium atoms per uranium atom on the surface of UO2, the best-fit value for the average number of uranium atoms indicates UO2 particles with an average diameter of 1.7 +/- 0.6 nm. The formation of nanometer-scale particles of UO2, suggested by the modeling of the EXAFS data, was confirmed by high-resolution transmission electron microscopy, which showed discrete particles (approximately 2-9 nm in diameter) of crystalline UO2. Our results clearly indicate that U(VI) (as soluble uranyl ion) is readily reduced by green rust to U(IV) in the form of relatively insoluble UO2 nanoparticles, suggesting that the presence of green rusts in the subsurface may have significant effects on the mobility of uranium, particularly under iron-reducing conditions.
Ferric Compounds↗
Military deployment human exposure assessment: urine total and isotopic uranium sampling results.
Currently the Department of Defense (DoD) does not use exposure biomarkers to measure service members' exposure to environmental chemicals. Blood and urine exposure biomarkers for volatile organic compounds (VOC), selected heavy metals, depleted uranium (DU), and chemical warfare agents are currently available but have not been field tested or validated by the DoD in military deployments as a tool to document exposures. The Military Deployment Human Exposure Assessment Study, a prospective cohort of 46 soldiers deployed to Bosnia, was designed to field test blood and urine exposure biomarkers as a mechanism to document exposures to these chemicals during military deployments. Blood and urine were collected before, during, and after deployment. Standard questionnaire, environmental, and occupational monitoring data collection methods were conducted for comparison to the exposure biomarker results. This article compares and reports the pre-, during, and postdeployment urine total and isotopic uranium measurements and compares them to perceived exposures captured on questionnaire, to environmental data collected by the United Nations Environmental Program in Bosnia, and to standard U.S. urine uranium reference levels (CDC, 2003). Additionally, the questionnaire and environmental and occupational measurements are reported. The results of the study indicate that exposure biomarkers may be a valuable tool to the DoD in exposure and risk assessment with regard to environmental and occupational exposures to uranium.
Bosnia and Herzegovina↗
Thermodynamic constraints on the oxidation of biogenic UO2 by Fe(III) (Hydr)oxides.
Uranium mobility in the environment is partially controlled by its oxidation state, where it exists as either U(VI) or U(IV). In aerobic environments, uranium is generally found in the hexavalent form, is quite soluble, and readily forms complexes with carbonate and calcium. Under anaerobic conditions, common metal respiring bacteria can reduce soluble U(VI) species to sparingly soluble UO2 (uraninite); stimulation of these bacteria, in fact, is being explored as an in situ uranium remediation technique. However, the stability of biologically precipitated uraninite within soils and sediments is not well characterized. Here we demonstrate that uraninite oxidation by Fe(III) (hydr)oxides is thermodynamically favorable under limited geochemical conditions. Our analysis reveals that goethite and hematite have a limited capacity to oxidize UO2(biogenic) while ferrihydrite can lead to UO2(biogenic) oxidation. The extent of UO2(biogenic) oxidation by ferrihydrite increases with increasing bicarbonate and calcium concentration, but decreases with elevated Fe(II)(aq) and U(VI)(aq) concentrations. Thus, our results demonstrate that the oxidation of UO2(biogenic) by Fe(III) (hydr)oxides may transpire under mildly reducing conditions when ferrihydrite is present.
Bacteria↗
Inhalation of U aerosols from UO2 fuel element fabrication.
Publication No. 30 of the International Commission on Radiological Protection (ICRP) assigns the uranium oxides UO2 and U3O8 to transportability class Y, i.e. the half-life of these compounds in the lungs is about 500 days. This assignment seemed not to be in accordance with our experience resulting from incorporation surveillance during UO2 fuel element fabrication. Persons who worked in atmospheres containing UO2 aerosols with activity concentrations significantly above the derived air concentrations (DAC) for class Y U showed much lower activity in the lungs than would be expected according to the ICRP. To understand this discrepancy, aerosol concentrations and aerosol particle-size distributions at work places with the possibility of UO2 incorporation, the activity of urine and feces and the lung activity of persons working at these places were measured in an investigation program. The results are only consistent with the ICRP lung model if one uses a measured biological half-life in the lungs of 109 days and a measured AMAD of 8.2 micron instead of the ICRP standard assumptions of 500 days and 1.0 micron, respectively. ICRP Publication No. 30 recommends application of specific parameters for health physics instead of standard model values. For the special conditions in our UO2 fuel fabrication plant we therefore derive limits of air concentrations, lung activities and fecal and urinary activity concentrations by applying our measured particle-size and lung-retention parameters to the ICRP model. Our special derived limits in comparison to class Y limits for U after ICRP Publication No. 30 for a 1-micron AMAD and 500-day half-life (in brackets) are: (a) annual limit of intake: 6 X 10(4) Bq/y (1 X 10(3) Bq/y); (b) derived air concentration: 20 Bq/m3 (0.6 Bq/m3); (c) derived lung activity: 1.6 X 10(3) Bq; (d) derived fecal activity: 14 Bq/day; and (e) derived urine activity: 8.9 Bq/day. The committed dose equivalents calculated from our measured data and from our modified derived limits proved consistent for the different incorporation control methods (determination of air concentration, lung, fecal or urinary activity). The authors recommend that in accordance with ICRP Publication No. 30, the national rules and regulations on activity incorporation provide the possibility to derive special limits from specific work-place parameters such as particle-size distributions and biological half-lives, thus supplementing the ICRP standard assumptions of 1 micron AMAD and biological half-lives of 0.5 days for class D, 50 days for class W and 500 days for class Y compounds.
Adult↗
Sister-chromatid exchanges in nuclear fuel workers.
Peripheral blood lymphocyte cultures of 116 smokers and 80 non-smokers who were occupationally exposed to uranyl compounds were analysed for sister-chromatid exchanges (SCEs). Blood samples were collected from 59 non-smokers (control group I) and 47 smokers (control group II) who were not exposed to uranium for control data. A significant increase in SCEs was observed among both smokers and non-smokers exposed to uranyl compounds when compared to their respective controls. In controls, a significant increase in the frequency of SCEs was observed in smokers when compared to non-smokers.
Adult↗
Water-insoluble Ag-U-organic assemblies with photocatalytic activity.
Two metal-organic coordination polymers [Ag(bipy)(UO(2))(bdc)(1.5)] (bipy=2,2'-bipyridyl, bdc=1,4-benzenedicarboxylate) and [Ag(2)(phen)(2)UO(2)(btec)] (phen=1,10-phenanthroline, btec=1,2,4,5-benzenetetracarboxylate) were obtained by hydrothermal assembly of the d(10) metal silver and the 5f metal uranium with mixed ligands. Both compounds form two-dimensional networks with pi-pi overlap interactions between the aromatic fragments in the neighboring layers. In aqueous suspension the two water-insoluble materials show photocatalytic degradation performance superior to that of commercial TiO(2) (Degussa P-25) when tested on nonbiodegradable rhodamine B (RhB) as model pollutant. The relationship between the structure of the photocatalysts and the photocatalytic activity was also elucidated. On the basis of the monitored intermediate species and the final mineralized products, it is proposed that the possible reaction mechanism for the photodegradation (oxidation) of RhB in aqueous solution catalyzed by the two assembly compounds involves photoexcitation of uranyl centers and molecular oxygen.
Journal Article↗
Syntheses of the Uranium Complexes [U{N(SiMe(3))(2)}(2){N(SiMe(3))(SiMe(2)CH(2)B(C(6)F(5))(3))}] and [U{C(Ph)(NSiMe(3))(2)}(2){&mgr;(3)-BH(4)}(2)]. Determination of Hydrogen Positions by Single-Crystal X-ray and Neutron Diffraction.
The complex [U{N(SiMe(3))(2)}(2){N(SiMe(3))(SiMe(2)CH(2)B(C(6)F(5))(3))}] (1) is formed in the reaction between the hydride complex [U{N(SiMe(3))(2)}(3)(H)] and B(C(6)F(5))(3), and H(2) is evolved. The X-ray [C(36)H(53)BF(15)N(3)Si(6)U.3.5C(6)D(6), triclinic, space group P&onemacr;, Z = 2, 90 K, a = 14.065(1) Å, b = 14.496(1) Å, c = 18.759(1) Å, alpha = 82.898(1) degrees, beta = 74.415(1) degrees, gamma = 62.919(1) degrees ] and neutron structure [C(36)H(53)BF(15)N(3)Si(6)U.3.5C(6)D(6), triclinic, space group P&onemacr;, Z = 2, 20 K, a = 13.993(1) Å, b = 14.484(1) Å, c = 18.720(1) Å, alpha = 82.810(1) degrees, beta = 74.200(1) degrees, gamma = 63.054(1)E] of compound 1, which crystallizes with 3.5 molecules of C(6)D(6) per asymmetric unit, show the electron deficiency of the uranium atom to be effectively compensated by the formation of multicenter bonds between U and three Si-CH(2) units of the amido ligands. The reaction of the uranium complex [U{C(Ph)(NSiMe(3))(2)}(2)(Cl)(2)] with [Na(BH(4))] gives the complex [U{C(Ph)(NSiMe(3))(2)}(2){&mgr;(3)-BH(4)}(2)] (2). The X-ray structure of 2 [C(26)H(54)B(2)N(4)Si(4)U, monoclinic, space group C2/c, Z = 4, 90 K, a = 21.613(1) Å, b = 9.233(1) Å, c = 18.132(1) Å, beta = 98.804(1) degrees ] proves unequivocally the &mgr;(3) coordination of the BH(4) moieties. In both single-crystal X-ray structure determinations, all hydrogen and deuterium atoms could be located and isotropically refined, including those which are directly coordinated to the uranium. The reliability of the refined hydrogen and deuterium positions for compound 1 is confirmed by comparison of the X-ray and neutron structure determinations. The ability to locate the hydrogen and deuterium positions in these uranium compounds by single-crystal X-ray diffraction is due to good crystal quality, the measurement of data at low temperature, and the use of image plate technology for data collection.
Journal Article↗
Efficacy of tiron for enhancing the excretion of uranium from the rat.
Tiron (sodium 4,5-dihydroxybenzene-1,3-disulphonate) has been suggested as a possible antidote for acute uranium poisoning. In this study, the compound has been administered intraperitoneally to rats in dosages of 30, 300 or 1000 mumols kg-1 at 20, 60 and 180 min after the intratracheal instillation of uranyl nitrate. The amounts of uranium deposited in the lungs of rats were equivalent to intakes by workers of about 12 times the permitted daily limit of 2.5 mg. The average body content of uranium at 5 d after exposure were, respectively, about 100%, 78% and 65% of those in untreated animals. It is concluded that the administration of Tiron is of limited practical value for treatment of uranium exposures not greatly in excess of the permitted intake.
1,2-Dihydroxybenzene-3,5-Disulfonic Acid Disodium ↗
Association of uranium with iron oxides typically formed on corroding steel surfaces.
Decontamination of metal surfaces contaminated with low levels of radionuclides is a major concern at Department of Energy facilities. The development of an environmentally friendly and cost-effective decontamination process requires an understanding of their association with the corroding surfaces. We investigated the association of uranium with the amorphous and crystalline forms of iron oxides commonly formed on corroding steel surfaces. Uranium was incorporated with the oxide by addition during the formation of ferrihydrite, goethite, green rust II, lepidocrocite, maghemite, and magnetite. X-ray diffraction confirmed the mineralogical form of the oxide. EXAFS analysis at the U L(III) edge showed that uranium was present in hexavalent form as a uranyl oxyhydroxide species with goethite, maghemite, and magnetite and as a bidentate inner-sphere complex with ferrihydrite and lepidocrocite. Iron was present in the ferric form with ferrihydrite, goethite, lepidocrocite, and maghemite; whereas with magnetite and green rust II, both ferrous and ferric forms were present with characteristic ferrous:total iron ratios of 0.65 and 0.73, respectively. In the presence of the uranyl ion, green rust II was converted to magnetite with concomitantreduction of uranium to its tetravalent form. The rate and extent of uranium dissolution in dilute HCl depended on its association with the oxide: uranium present as oxyhydroxide species underwent rapid dissolution followed by a slow dissolution of iron; whereas uranium present as an inner-sphere complex with iron resulted in concomitant dissolution of the uranium and iron.
Corrosion↗
The effects of repeated parenteral administration of chelating agents on the distribution and excretion of uranium.
The effects of repeated ip administration of gallic acid, 4,5-dihydroxy-1,3-benzenedisulfonic acid (Tiron), diethylenetriaminepentaacetic acid (DTPA), and 5-aminosalicylic acid (5-AS) on the distribution and excretion of uranium were assessed in male Swiss mice. Only Tiron significantly increased the amount of uranium excreted into urine and feces. A significant decrease in the concentration of uranium in liver, spleen and bone was observed after administration of Tiron, whereas injection of gallic acid or DTPA resulted in a significant decrease in the concentration of the metal in the liver. The results show that Tiron was consistently the most effective chelator of those tested in the treatment of uranium poisoning after repeated daily administration of the metal.
Animals↗
Reactions of salicylate with uranium(VI) and cobalt(II)-allylamine complex. Micro detection of uranium(VI) and salicylate.
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Allyl Compounds↗
The effect of uranyl acetate on human lymphoblastoid cells (RPMI 6410) and HeLa cells.
RPMI 6410 cells and HeLa cells were exposed to uranyl acetate. In RPMI 6410 cell cultures this produced single-membrane-bound presumably lysosomal bodies (called "uraniosomes") containing electron-dense crystals in the cultured cells and crystalline deposits in extracellular locations. Neither uraniosomes nor extracellular uranium deposits were found in HeLa cell cultures. All uraniosomes and extracellular uranium deposits analysed by electron-probed X-ray analysis were found to contain uranium, potassium and phosphorus. Traces of sulphur were detected in some but not all uraniosomes and extracellular uranium deposits. Traces of calcium were found in all extracellular uranium deposits and in some uraniosomes also.
Calcium↗
Ferric acetate-uranium acetate reagent in cholesterol estimations in plasma and high density lipoprotein fractions: comparison with existing methods.
The use of ferric acetate-uranium acetate colour reaction for the estimation of cholesterol in the supernatants of plasma samples after precipitation of low density lipoprotein (LDL) and very low density lipoprotein (VLDL) cholesterol by heparin-MnCl2 was assessed and compared with the conventional method using the FeCl3 colour reaction and also with the method using o-phthalaldehyde as the colouring reagent. All three methods gave comparable values when total cholesterol in plasma samples was determined and also when high density lipoprotein (HDL) fractions were separated by ultracentrifugation and the cholesterol contents determined. But when heparin-MnCl2 precipitation was used for HDL separation, and the cholesterol content determined, the FeCl3 method gave significantly lower values. This could be due to interference of the cholesterol colour reaction with FeCl3, due to Mn2+ ions present in the supernatant. Addition of Mn2+ to cholesterol standards and subsequent colour development with ferric acetate-uranium acetate and FeCl3 reagents showed that Mn2+ decreased the absorbancy of the coloured complex at 560 nm only when FeCl3 was used. Percentage recovery of added cholesterol was also lower when the heparin-MnCl2 supernatant was treated with FeCl3 reagent for colour development. Use of ferric acetate-uranium acetate reagent provides a simpler and quicker method. It does not suffer from interference due to the presence of Mn2+ ions and gives results comparable to the o-phthalaldehyde method and those using ultracentrifugation as the separation procedure.
Chemical Precipitation↗
Chelation of UO(2)(2+) by vitamin B6 complex derivatives: synthesis and characterization of [UO2(beta-pyracinide)2(H2O)] and [UO2(Pyr2en)DMSO]Cl2{Pyr2en=N,N'-ethylenebis(pyridoxylideneiminato)}. A useful modeling of assimilation of uranium by living beings.
The vitamin B(6) derivatives 4-pyridoxic acid (anionic) and the Schiff base N,N'-ethylenebis(pyridoxylideneiminato) react with UO(2)(NO(3))(2) * 6H(2)O to give [UO(2)(beta-pyracinide)(2)(H(2)O)] (beta-pyracin=4-pyridoxic acid) and [UO(2)(Pyr(2)en)DMSO]Cl(2)(Pyr(2)en=N,N'-ethylenebis(pyridoxylideneiminato); DMSO=dimethyl sulfoxide). In both compounds the two uranyl oxo ligands set the axis of distorted pentagonal bipyramides. The ability of vitamin B(6) derivatives to react with UO(2)(2+) allowing the chelation of one uranium atom represents a very specific model of assimilation of uranium by living beings. It could also explain the serious damages caused by heavy or radioactive metals like uranium since their complexation "in vivo" by enzymatic systems like pyridoxal phosphate-containing enzymes would lead to a modification of the prosthetic groups of the metalloenzymes with loss of their catalytic activities.
Chelating Agents↗
Biological and chemical interactions with U(VI) during anaerobic enrichment in the presence of iron oxide coated quartz.
Microcosm experiments were performed to understand chemical and biological interactions with hexavalent uranium (U(VI)) in the presence of iron oxide bearing minerals and trichloroethylene (TCE) as a co-contaminant. Interactions of U(VI) and hydrous iron oxide moieties on the mineral oxide surfaces were studied during enrichments for dissimilatory iron reducing (DIRB) and sulfate reducing bacteria (SRB). Microbes enriched from groundwater taken from the Test Area North (TAN) site at the Idaho National Laboratory (INL) were able to reduce the U(VI) in the adsorption medium as well as the iron on quartz surfaces. Early in the experiment disappearance of U(VI) from solution was a function of chemical interactions since no microbial activity was evident. Abiotic removal of U(VI) was enhanced in the presence of carbonate. As the experiment proceeded, further removal of U(VI) from solution was associated with the fermentation of lactate to propionate and acetate. During later phases of the experiment when lactate was depleted from the growth medium in the microcosm containing the DIRB enrichments, U(VI) concentrations in the solution phase increased until additional lactate was added. When additional lactate was added and fermentation proceeded, U(VI) concentrations in the liquid phase again returned to near zero. Similar results were shown for the SRB enrichment but lower uranium concentrations were seen in the liquid phase, while in the enrichment with carbonate a similar increase in uranium concentration was not seen. Chemical and biological interactions appear to be important on the mobilization/immobilization of U(VI) in an iron oxide system when TCE is present as a co-contaminant. Interestingly, TCE present in the microcosm experiments was not dechlorinated which was probably an effect of redox conditions that were unsuitable for reductive dechlorination by the microbial culture tested.
Adsorption↗
Metabolism of some industrial uranium tetrafluorides after deposition in the rat lung.
UNLABELLED: Two commercially produced natural uranium tetrafluorides were administered to rats either by inhalation or direct injection into the lungs. THE RESULTS: show that, for both materials uranium is cleared rapidly from the lungs, much of it to the blood, show that the distribution of uranium amongst body tissues, and the fraction of the systemic content excreted in urine, is similar to that obtained after the administration of U(VI) bicarbonate, show that the transportability of uranium is much greater than in previously reported studies with other preparations of uranium tetrafluoride, suggest that lung radioactivity counting measurements would be of limited value for interpreting human exposures, indicate that for setting exposure limits these tetrafluorides should be considered moderately transportable compounds (ICRP inhalation class W).
Animals↗
Synthesis and structure of diamido ether uranium(IV) and thorium(IV) halide "ate" complexes and their conversion to salt-free bis(alkyl) complexes.
The high-yield synthesis, spectroscopic and structural determination of three new uranium(IV) and thorium(IV)ate complexes supported by three different diamido ether ligands are reported. The reaction of Li2[2,6-iPr2PhN(CH2CH2)]2O (Li2[DIPPNCOCN]) with 1 equiv. of UCl4 in THF generates [DIPPNCOCN]UCl3Li(THF)2(1), while reaction in toluene/ether gives salt-free [DIPPNCOCN]UCl2.1/2C7H8(2), which was identified by paramagnetically shifted 1H NMR. Reaction of 0.5 equiv. of {[tBuNON]UCl2}2([tBuNON]=[(CH3)3CN(Si(CH3)2)]2O2-) with 3.5 equiv. LiI in toluene and a minimal amount of THF results in [tBuNON]UI3Li(THF)2(3) and is very similar in structure to 1. {[MesNON]ThCl3Li(THF)}2(4), a dimeric complex with a Th2Li2Cl6 core, is prepared by reaction of Li2[2,4,6-Me3PhN(Si(CH3)2)]2O (Li2[MesNON]) with ThCl4 in THF. The analogous reaction in toluene did not yield the salt-free complex but rather a sterically crowded diligated compound, [MesNON]2Th (5), which was also structurally characterized. Complex 5 was prepared rationally by reacting 2 equiv. Li2[MesNON] with ThCl4 in toluene. The reaction of 1 and 3 with 2 equiv. of LiCH2Si(CH3)3 generates the stable, salt-free organoactinides [DIPPNCOCN]U(CH2Si(CH3)3)2(6) and [tBuNON]U(CH2Si(CH3)3)2(7). Complex 6 was structurally characterized. These reactions illustrate the viability of ate complexes as useful synthetic precursors.
Chlorides↗