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Pu(V) reduction and enhancement of particle-water partitioning by exopolymeric substances
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Kimberly A. Roberts
Veröffentlicht/Copyright:
25. September 2009
Abstract
Central to understanding the environmental behavior of Pu in vadose- and saturated-zones, as well as waste streams, is the contribution of colloidal natural organic mater (NOM), e.g. , biopolymeric exopolymeric substances (EPS) from Pseudomonas fluorescens Biovar II and geopolymeric humic acids (HA), to Pu speciation. Because Pu(V) and Pu(IV) are present in aquatic systems at sub-pM concentrations, many established techniques for chemical speciation and oxidation state determination are not available. However, the two redox states of Pu can be distinguished through their tendency to form colloidal species. Controlled laboratory experiments with low-colloid background solutions of 0.1 M NaClO4 with an inert buffer (Tris) and 5 μm silica particles of high specific surface area (500 m2/g) and small (3 nm) pores investigated the ability of NOM compounds for their binding and redox qualities showed that: 1) Pu(V) and Pu(IV) tracers at pM concentrations could be distinguished by their tendency to bind to colloidal species (≥1 kDa), with binding extent being high for Pu(IV), and low for Pu(V); 2) EPS can significantly enhance particle- (or colloid-) water partition coefficients to silica particles (Kd, Kdc), quickly (1 day) for Pu(IV) and slowly (1 month) for Pu(V); 3) Pu(V), in the presence of EPS and silica particles can become associated with particles and colloids over periods of months, likely indicating reduction; 4) Kd values can be affected by the reaction sequence of tracer addition to the solution containing silica particles and NOM compounds ( e.g. , EPS or HA).
Published Online: 2009-09-25
Published in Print: 2008-11
© by Oldenbourg Wissenschaftsverlag, -1887 Golden, 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
Schlagwörter für diesen Artikel
Plutonium;
Pu(V) reduction;
Pu(IV);
Thorium;
Particle-water partitioning
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
