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PubMed2002

NMR shielding calculations across the periodic table: diamagnetic uranium compounds. 2. Ligand and metal NMR.

In this and a previous article (J. Phys. Chem. A 2000, 104, 8244), the range of application for relativistic density functional theory (DFT) is extended to the calculation of nuclear magnetic resonance (NMR) shieldings and chemical shifts in diamagnetic actinide compounds. Two relativistic DFT methods are used, ZORA ("zeroth-order regular approximation") and the quasirelativistic (QR) method. In the given second paper, NMR shieldings and chemical shifts are calculated and discussed for a wide range of compounds. The molecules studied comprise uranyl complexes, [UO(2)L(n)](+/-)(q); UF(6); inorganic UF(6) derivatives, UF(6-n)Cl(n), n = 0-6; and organometallic UF(6) derivatives, UF(6-n)(OCH(3))(n), n = 0-5. Uranyl complexes include [UO(2)F(4)](2-), [UO(2)Cl(4)](2-), [UO(2)(OH)(4)](2-), [UO(2)(CO(3))(3)](4-), and [UO(2)(H(2)O)(5)](2+). For the ligand NMR, moderate (e.g., (19)F NMR chemical shifts in UF(6-n)Cl(n)) to excellent agreement [e.g., (19)F chemical shift tensor in UF(6) or (1)H NMR in UF(6-n)(OCH(3))(n)] has been found between theory and experiment. The methods have been used to calculate the experimentally unknown (235)U NMR chemical shifts. A large chemical shift range of at least 21,000 ppm has been predicted for the (235)U nucleus. ZORA spin-orbit appears to be the most accurate method for predicting actinide metal chemical shifts. Trends in the (235)U NMR chemical shifts of UF(6-n)L(n) molecules are analyzed and explained in terms of the calculated electronic structure. It is argued that the energy separation and interaction between occupied and virtual orbitals with f-character are the determining factors.

Journal Article↗
PubMed2004

Model results of kidney burdens from uranium intakes.

Uranium is a naturally occurring element, which is both radiologically and chemically toxic. When dealing with intakes of uranium, whether natural or depleted, chemical toxicity to the kidney usually predominates over radiological toxicity. This is especially true for uranium compounds in soluble (inhalation Type F) and moderately soluble (inhalation Type M) forms. To assess chemical toxicity, information on kidney burden per unit intake is required. This study summarizes the kidney burdens per unit intake for common exposures from uranium ingestion and inhalation. ICRP models developed for radiation dosimetry purposes can equally well be used to estimate kidney burdens from uranium intakes. While dosimetric quantities and data are tabulated in ICRP publications, data on uranium burdens in kidney are not explicitly given in these tabulations. In this work, the most recent ICRP models were utilized to generate a compilation of kidney burdens from common intakes. Calculations were made for four age groups from infant to adult. For all age groups, long-term chronic uranium ingestion will result in a kidney burden of 6.6% of daily uranium intake. Comparisons of kidney burdens due to acute ingestion and acute inhalation show that inhaled uranium compounds of Type F and Type M will generally result in higher burdens to kidney compared to the same amount of uranium compounds ingested.

Administration, Inhalation↗
PubMed2006

Distribution and genotoxic effects after successive exposure to different uranium oxide particles inhaled by rats.

In nuclear fuel cycle facilities, workers may inhale airborne uranium compounds that lead to internal contamination, with various exposure scenarios depending on the workplace. These exposures can be chronic, repeated, or acute, and can involve many different compounds. The effect of uranium after multiple scenarios of exposure is unknown. The aim of this study, therefore, was to investigate the genotoxic and biokinetics consequences of exposure to depleted insoluble uranium dioxide (UO2) by repeated or acute inhalation on subsequent acute inhalation of moderately soluble uranium peroxide (UO4) in rats. The results show that UO2 repeated preexposure by inhalation increases the genotoxic effects of UO4 inhalation, assessed by comet assay, in different cell types, when UO4 exposure alone has no effect. At the same time, the study of UO4 bioaccumulation showed that the UO4 biokinetics in the kidneys, gastrointestinal tract, and excreta, but not in the lungs, were slightly modified by previous UO2 exposures. All these results show that both genotoxic and biokinetics effects of uranium may depend on preexposure and that repeated exposure induces a potentiation effect compared with acute exposure.

Aerosols↗
PubMed2003

Comparative reactivity of sterically crowded nf3 (C5Me5)3Nd and (C5Me5)3U complexes with CO: formation of a nonclassical carbonium ion versus an f element metal carbonyl complex.

Sterically crowded isoelectronic nf(3) (C(5)Me(5))(3)M complexes of neodymium and uranium, compounds which have unconventionally long metal ligand distances, are found to react very differently with CO as a substrate. The 4f(3) complex (C(5)Me(5))(3)Nd reacts with CO to form a nonclassical carbonium ion complex, (C(5)Me(5))(2)Nd(O(2)C(7)Me(5)), which contains a three-coordinate planar carbon. (C(5)Me(5))(3)U reacts with CO to form an even more crowded CO adduct through a reaction type never observed before for (C(5)Me(5))(3)M compounds. The rare uranium carbonyl complex, (C(5)Me(5))(3)U(CO), has nu(CO) = 1922 cm(-1) and a U-C(CO) distance of 2.485(9) A.

Journal Article↗
PubMed2006

Uranium induces oxidative stress in lung epithelial cells.

Uranium compounds are widely used in the nuclear fuel cycle, antitank weapons, tank armor, and also as a pigment to color ceramics and glass. Effective management of waste uranium compounds is necessary to prevent exposure to avoid adverse health effects on the population. Health risks associated with uranium exposure includes kidney disease and respiratory disorders. In addition, several published results have shown uranium or depleted uranium causes DNA damage, mutagenicity, cancer and neurological defects. In the current study, uranium toxicity was evaluated in rat lung epithelial cells. The study shows uranium induces significant oxidative stress in rat lung epithelial cells followed by concomitant decrease in the antioxidant potential of the cells. Treatment with uranium to rat lung epithelial cells also decreased cell proliferation after 72 h in culture. The decrease in cell proliferation was attributed to loss of total glutathione and superoxide dismutase in the presence of uranium. Thus the results indicate the ineffectiveness of antioxidant system's response to the oxidative stress induced by uranium in the cells.

Acetylcysteine↗
PubMed1998

Halide Effects in the Synthesis of Mixed Uranium(IV) Aryloxide-Halide Compounds.

Several uranium(IV) aryloxide and mixed aryloxide-halide compounds of the formula UX(4)(-)(z)()(OAr)(z)() (X = Cl, Br, I; OAr = 2,6-di-tert-butylphenoxide; z = 2, 3, 4) have been prepared by the reaction of KOAr with the appropriate uranium tetrahalide in tetrahydrofuran (THF). The complex UI(4)(CH(3)CN)(4) reacts with 2 equiv of KOAr in THF to yield the compound I(2)U(OAr)(2) (1). The utility of this reaction is limited by the instability of UI(4)(CH(3)CN)(4) in THF, however, and isolated yields of the THF adduct of 1 do not exceed 50%. In contrast, UBr(4)(CH(3)CN)(4) is stable in THF solution and reacts with 2 equiv of KOAr to yield the dibromide, Br(2)U(OAr)(2)(THF) (4.THF), in 77% yield. Under identical reaction conditions, UCl(4) reacts to yield the complex [K(THF)(4)][UCl(3)(OAr)(2)] (5) in 68% yield. The uranium center in compound 5 is coordinated by two trans aryloxide ligands and three chloride ligands in a trigonal bipyramidal arrangement. Two chloride ligands of each unit are also coordinated to a potassium ion, forming an infinite chain in the lattice. Compounds 1 and 5 will further react with 1 equiv of KOAr to yield the compounds XU(OAr)(3) (2, X = I; 6, X = Cl). Both UI(4)(CH(3)CN)(4) and UCl(4) will react with a 4.2 equiv of KOAr to yield the previously characterized compound U(OAr)(4) (3). The stability of the mixed aryloxide-halide uranium complexes toward ligand redistribution reactions has been investigated.

Journal Article↗