Measurements and modelling of Pm sorption onto TiO2 and goethite
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Anna-Maria Jakobsson
Summary
The sorption of Pm (1×10-9 M) onto TiO2 and goethite has been studied as a function of pH and ionic strength (0.01, 0.1 M NaClO4) at ambient temperature under N2 atmosphere. For both minerals studied there is no effect of the different ionic strengths and the sorption (log Kavs. pH) increases with a slope of ∼2. At the same pH sorption is lower on the more positively (or less negatively) charged goethite (pHpzc=8.4) than on the TiO2 (pHpzc=6.2). A comparison to other trivalent cations sorbed on different substrates (made by extracting values from %-sorbed curves and calculating these to Ka) indicate a similar pH-dependence.
The results have been fitted using a 1-pK basic Stern model with FITEQL. An a priori restriction was that only one sorption reaction stoichiometry at a time was to be used to keep the number of parameters as small as possible. Outer-sphere and mono-, bi- and tri-dentate inner-sphere complexes were fitted. For each fit the value of the capacitance was varied to find the value that provided the best fit. Two different site densities were used: 1 site/nm2 and 2.31 sites/nm2. For the low site density the reaction which provides the best fit was:
≡SOH0.5-+Pm+3↔≡SOHPm2.5+
for both minerals. At the high site density the same reaction fits for TiO2 while there are several reactions that are equivalent in the fit for goethite.
© 2004 Oldenbourg Wissenschaftsverlag GmbH
Artikel in diesem Heft
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- Actinide chemistry: from weapons to remediation to stewardship
- Thermodynamics and solubility of (UxNp1-x)O2(am) solid solution in the carbonate system
- Solubility and colloid formation of Th(IV) in concentrated NaCl and MgCl2 solution
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- Contribution of minerals to the sorption of U(VI) on granite
- Distribution and geochemical association of actinides in a contaminated soil as a function of grain size
- Interactions between anionic complex species of actinides and negatively charged mineral surfaces
- Measurements and modelling of Pm sorption onto TiO2 and goethite
- Effect of humic acid on the sorption of Cm(III) onto γ-Al2O3 studied by the time-resolved laser fluorescence spectroscopy
- Am(III) and Eu(III) uptake on hematite in the presence of humic acid
- Luminescence properties of tetravalent uranium in aqueous solution
- Scanning transmission X-ray microscopy as a speciation tool for natural organic molecules
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- Results of the colloid and radionuclide retention experiment (CRR) at the Grimsel Test Site (GTS), Switzerland – impact of reaction kinetics and speciation on radionuclide migration
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- Comparison between in situ and laboratory diffusion studies of HTO and halides in Opalinus Clay from the Mont Terri
- Solubility constraints on uranium concentrations in groundwaters of the Tono uranium deposit, Japan
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- Towards a common thermodynamic database for speciation models
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Artikel in diesem Heft
- Preface: Migration Conference 2003
- Actinide chemistry: from weapons to remediation to stewardship
- Thermodynamics and solubility of (UxNp1-x)O2(am) solid solution in the carbonate system
- Solubility and colloid formation of Th(IV) in concentrated NaCl and MgCl2 solution
- Effect of reducing agents on the uranium concentration above uranium(IV) amorphous precipitate in Boom Clay pore water
- On Mo-Ru-Tc-Pd-Rh-Te alloy particles extracted from spent fuel and their leaching behavior under Ar and H2 atmospheres
- Modeling of the complex formation of metal ions with humic acids
- Application of the NICA-Donnan model for proton, copper and uranyl binding to humic acid
- Protonation and complexation of isosaccharinic acid with U(VI) and Fe(III) in acidic solutions: potentiometric and calorimetric studies
- Carbonate complexation of neptunium(IV) in highly basic solutions
- Fluorescence characteristics of complex formation of europium(III)-salicylate
- The reduction of U(VI) by near field hydrogen in the presence of UO2(s)
- Electrochemical aspects of radiolytically enhanced UO2 dissolution
- Effect of alpha radiolysis on doped UO2 dissolution under reducing conditions
- The redox behaviour of plutonium in humic rich groundwater
- The fate of radiolytic oxidants during spent fuel leaching in the presence of dissolved near field hydrogen
- Structural changes of uranyl moiety with reduction from U(VI) to U(V)
- Trivalent actinide coprecipitation with powellite (CaMoO4): Secondary solid solution formation during HLW borosilicate-glass dissolution
- Reproducibility of the uptake of U(VI) onto degraded cement pastes and calcium silicate hydrate phases
- Uranium adsorption on weathered schist – intercomparison of modelling approaches
- Contribution of minerals to the sorption of U(VI) on granite
- Distribution and geochemical association of actinides in a contaminated soil as a function of grain size
- Interactions between anionic complex species of actinides and negatively charged mineral surfaces
- Measurements and modelling of Pm sorption onto TiO2 and goethite
- Effect of humic acid on the sorption of Cm(III) onto γ-Al2O3 studied by the time-resolved laser fluorescence spectroscopy
- Am(III) and Eu(III) uptake on hematite in the presence of humic acid
- Luminescence properties of tetravalent uranium in aqueous solution
- Scanning transmission X-ray microscopy as a speciation tool for natural organic molecules
- Formation of hydroxyapatite in soils using calcium citrate and sodium phosphate for control of strontium migration
- Influence of humic substances on the 63Ni migration through crushed rock media
- U, Th, Eu and colloid mobility in a granite fracture under near-natural flow conditions
- Sorption behavior of europium(III) and curium(III) on the cell surfaces of microorganisms
- Interactions of trivalent and tetravalent heavy metal-siderophore complexes with Pseudomonas fluorescens
- In-situ diffusion of HTO, 22Na+, Cs+ and I- in Opalinus Clay at the Mont Terri underground rock laboratory
- Results of the colloid and radionuclide retention experiment (CRR) at the Grimsel Test Site (GTS), Switzerland – impact of reaction kinetics and speciation on radionuclide migration
- Fracture flow and radionuclide transport in block-scale laboratory experiments
- Comparison between in situ and laboratory diffusion studies of HTO and halides in Opalinus Clay from the Mont Terri
- Solubility constraints on uranium concentrations in groundwaters of the Tono uranium deposit, Japan
- Mobility of uranium in tertiary argillaceous sediments – a natural analogue study
- Redistribution of U, Pb and REE in association with alteration of uranium minerals from the Koongarra deposit, Northern Territory, Australia
- Towards a common thermodynamic database for speciation models
- Geochemically derived non-gaseous radionuclide source term for the Asse salt mine – assessment for the use of a Mg(OH)2-based backfill material
- Simulation of remediation alternatives for a 137Cs contaminated soil
- Simulating reactive transport in time dependent multiphase flow problems
- Reactive transport modelling of a spent fuel repository in a stiff clay formation considering excavation damaged zones
- Coupled transport/reaction modelling of copper canister corrosion aided by microbial processes