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Mechanisms of plutonium sorption to mineral oxide surfaces: new insights with implications for colloid-enhanced migration
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J. M. Schwantes
Published/Copyright:
November 23, 2010
Abstract
New equilibrium and kinetic models have been developed to describe rate-limited sorption and desorption of Pu onto and off of mineral oxide surfaces using a generic approach to estimate sorption constants that require minimal laboratory calibrations. Equilibrium reactions describing a total of six surface species were derived from a combination of empirical relationships previously described in the literature and generated as part of this work. These sorption reactions and corresponding equilibrium constants onto goethite (and silica) are:
≡SOH + Pu3+ ↔ ≡SOPu2+ + H+, logߙK = −2.1(−10) (1)
≡SOH + Pu4+ ↔ ≡SOPu3+ + H+, logߙK = 15.3(7.2) (2)
≡SOH + PuO2+ ↔ ≡SOPuO2 + H+, logߙK = −8.5(−16.5) (3)
≡SOH + PuO22+ ↔ ≡SOPuO2+ + H+, logߙK = 1.2(−6.5) (4)
≡SOH + Pu4+ + 3H2O ↔ ≡SOPu(OH)3 + 4H+, logߙK = 12.5(4.6) (5)
≡SOH + Pu4+ + 4H2O ↔ ≡SOPu(OH)4− + 5H+, logߙK = 5.0(−2.3) (6)
The kinetic model decouples reduced (III, IV) and oxidized (V, VI) forms of Pu via a single rate-limiting, but reversible, surface mediated reaction:...
Published Online: 2010-11-23
Published in Print: 2010-11
© by Oldenbourg Wissenschaftsverlag, Richland, WA 99352, Germany
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- Preface
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- Chlorine speciation in nuclear graphite: consequences on temperature release and on leaching
- Chemical status of U(VI) in cemented waste forms under saline conditions
- Influence of iron redox transformations on plutonium sorption to sediments
- Modelling of a large-scale in-situ migration experiment with 14C-labelled natural organic matter in Boom Clay
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Articles in the same Issue
- Preface
- Solubility of tetravalent actinides in alkaline CaCl2 solutions and formation of Ca4[An(OH)8]4+ complexes: A study of Np(IV) and Pu(IV) under reducing conditions and the systematic trend in the An(IV) series
- Solubility of triuranyl diphosphate tetrahydrate (TDT) and Na autunite at 23 and 50 °C
- Effect of reduction on the stability of Pu(VI) hydrolysis species
- Retention and redox behaviour of uranium(VI) by siderite (FeCO3)
- Neptunium(V) complexation by natural pyoverdins and related model compounds
- Complexation of Nd(III) with tetraborate ion and its effect on actinide(III) solubility in WIPP brine
- Complexation of Tc(IV) with acetate at varying ionic strengths
- Uranyl photochemistry: decarboxylation of gluconic acid
- Influence of Boom Clay organic matter on the adsorption of Eu3+ by illite – geochemical modelling using the component additivity approach
- The role of green rust in the migration of radionuclides: An overview of processes that can control mobility of radioactive elements in the environment using as examples Np, Se and Cr
- A comparative batch sorption and time-resolved laser fluorescence spectroscopy study on the sorption of Eu(III) and Cm(III) on synthetic and natural kaolinite
- U(VI) sorption on granite: prediction and experiments
- Quantum chemical study of inner-sphere complexes of trivalent lanthanide and actinide ions on the corundum (0001) surface
- Quantum chemical modeling of uranyl adsorption on mineral surfaces
- Interaction of PuO2 thin films with water
- Molecular interactions of plutonium(VI) with synthetic manganese-substituted goethite
- Chlorine speciation in nuclear graphite: consequences on temperature release and on leaching
- Chemical status of U(VI) in cemented waste forms under saline conditions
- Influence of iron redox transformations on plutonium sorption to sediments
- Modelling of a large-scale in-situ migration experiment with 14C-labelled natural organic matter in Boom Clay
- Sorption and diffusion of Eu in sedimentary rock in the presence of humic substance
- Diffusion and sorption of neptunium(V) in compacted montmorillonite: effects of carbonate and salinity
- Uranium(VI) diffusion in low-permeability subsurface materials
- Distribution of Cs and Am in the solution-bentonite colloids-granite ternary system: effect of addition order and sorption reversibility
- Mechanisms of plutonium sorption to mineral oxide surfaces: new insights with implications for colloid-enhanced migration
- Understanding uranium behaviour at the Askola uranium mineralization
