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A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
-
Zheming Wang
Veröffentlicht/Copyright:
25. September 2009
Abstract
In this paper, the reduction rate of uranyl complexes with hydroxide, carbonate, EDTA, and desferriferrioxamine B (DFB) by anthraquinone-2,6-disulfonate (AH2DS) is studied by stopped-flow kinetic technique under anoxic atmosphere. The apparent reaction rates varied with ligand type, solution pH, and U(VI) concentration. For each ligand, a single largest pseudo −1st order reaction rate constant, kobs, within the studied pH range was observed, suggesting the influence of pH-dependent speciation on the U(VI) reduction rate. The maximum reaction rate found in each case followed the order of OH−>CO32−>EDTA>DFB, in reverse order of the trend of the thermodynamic stability of the uranyl complexes and ionic sizes of the ligands. The pH-dependent rates were modeled using a second-order rate expression that was assumed to be dependent on a single U(VI) complex and an AH2DS species. By quantitatively comparing the calculated and measured apparent rate constants as a function of pH, species AHDS3− was suggested as the primary reductant in all cases examined. Species UO2CO3(aq), UO2HEDTA−, and (UO2)2(OH)22+ were suggested as the principal electron acceptors among the U(VI) species mixture in each of the carbonate, EDTA, and hydroxyl systems, respectively.
Published Online: 2009-09-25
Published in Print: 2008-11
© by Oldenbourg Wissenschaftsverlag, Richland, Germany
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Artikel in diesem Heft
- Preface
- Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface
- Modeling plutonium solubility for Yucca Mountain performance assessment
- Uranium/technetium separation for the UREX process – synthesis and characterization of solid reprocessing forms
- UO2 dissolution in the presence of hydrogen peroxide at pH>11
- Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes
- A TRLFS study of Cm(III) hydroxide complexes in alkaline CaCl2 solutions
- Thermodynamic interpretation of neptunium coprecipitation in uranophane for application to the Yucca Mountain repository
- Structural investigation of coprecipitation of technetium-99 with iron phases
- Synthesis, crystallographic characterization, and conformational prediction of a structurally unique molecular mixed-ligand U(VI) solid, Na6[UO2(O2)2(OH)2](OH)2·14H2O
- Thermodynamic study on the U(VI) complexation with dicarboxylates by calorimetry
- A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals
- A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
- The relationship of monodentate and bidentate coordinated uranium(VI) sulfate in aqueous solution
- Hydrolysis constants of tetravalent neptunium by using solvent extraction method
- Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation
- Oxidative dissolution of Tc(IV)O2·nH2O colloids by sonolysis
- Technetium reduction and reoxidation behaviour in Dounreay soils
- Effects of hydrogen and bromide on the corrosion of spent nuclear fuel and γ-irradiated UO2(s) in NaCl brine
- Sorption of selenium on Mg-Al and Mg-Al-Eu layered double hydroxides
- Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
- Polarized EXAFS characterization of the sorption mechanism of yttrium on hectorite
- Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
- Hydration and hydrolysys of Sm3+ and Eu3+ in a clay interlayer: a neutron diffraction study with isotopic substitution
- Sorption of neptunium onto goethite in the presence of humic acids with different hydroquinone group content
- The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
- Sorption of radionuclides onto natural clay rocks
- The influence of natural organic matter on the speciation and solubility of Eu in Boom Clay porewater
- Sorption behavior of americium onto bentonite colloid
- Vertical distribution of 238Pu, 239(40)Pu, 241Am, 90Sr and 137Cs in Austrian soil profiles
- Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
- Laser ablation microprobe inductively coupled plasma mass spectrometry study on diffusion of uranium into cement materials
- Binding of Pu(IV) to galacturonic acid and extracellular polymeric substances (EPS) from Shewanella putrefaciens, Clostridium sp. and Pseudomonas fluorescens
Artikel in diesem Heft
- Preface
- Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface
- Modeling plutonium solubility for Yucca Mountain performance assessment
- Uranium/technetium separation for the UREX process – synthesis and characterization of solid reprocessing forms
- UO2 dissolution in the presence of hydrogen peroxide at pH>11
- Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes
- A TRLFS study of Cm(III) hydroxide complexes in alkaline CaCl2 solutions
- Thermodynamic interpretation of neptunium coprecipitation in uranophane for application to the Yucca Mountain repository
- Structural investigation of coprecipitation of technetium-99 with iron phases
- Synthesis, crystallographic characterization, and conformational prediction of a structurally unique molecular mixed-ligand U(VI) solid, Na6[UO2(O2)2(OH)2](OH)2·14H2O
- Thermodynamic study on the U(VI) complexation with dicarboxylates by calorimetry
- A cryogenic fluorescence spectroscopic study of uranyl carbonate, phosphate and oxyhydroxide minerals
- A spectroscopic study of the effect of ligand complexation on the reduction of uranium(VI) by anthraquinone-2,6-disulfonate (AH2DS)
- The relationship of monodentate and bidentate coordinated uranium(VI) sulfate in aqueous solution
- Hydrolysis constants of tetravalent neptunium by using solvent extraction method
- Leaching of a zirconolite ceramic waste-form under proton and He2+ irradiation
- Oxidative dissolution of Tc(IV)O2·nH2O colloids by sonolysis
- Technetium reduction and reoxidation behaviour in Dounreay soils
- Effects of hydrogen and bromide on the corrosion of spent nuclear fuel and γ-irradiated UO2(s) in NaCl brine
- Sorption of selenium on Mg-Al and Mg-Al-Eu layered double hydroxides
- Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)
- Polarized EXAFS characterization of the sorption mechanism of yttrium on hectorite
- Measuring sorption coefficients and BET surface areas on intact drillcore and crushed granite samples
- Hydration and hydrolysys of Sm3+ and Eu3+ in a clay interlayer: a neutron diffraction study with isotopic substitution
- Sorption of neptunium onto goethite in the presence of humic acids with different hydroquinone group content
- The influence of carbonate complexation on lanthanide/actinide sorption on montmorillonite
- Sorption of radionuclides onto natural clay rocks
- The influence of natural organic matter on the speciation and solubility of Eu in Boom Clay porewater
- Sorption behavior of americium onto bentonite colloid
- Vertical distribution of 238Pu, 239(40)Pu, 241Am, 90Sr and 137Cs in Austrian soil profiles
- Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
- Laser ablation microprobe inductively coupled plasma mass spectrometry study on diffusion of uranium into cement materials
- Binding of Pu(IV) to galacturonic acid and extracellular polymeric substances (EPS) from Shewanella putrefaciens, Clostridium sp. and Pseudomonas fluorescens
