Reproducibility of the uptake of U(VI) onto degraded cement pastes and calcium silicate hydrate phases
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I. Pointeau
Abstract
The U(VI) uptake in degraded cement pastes was undertaken in the laboratories of CEA/L3MR and SUBATECH in order to check the reproducibility of the study. Two well hydrated cement pastes, CEM I (Ordinary Portland Cement, OPC) and CEM V (blast furnace slag (BFS) and fly ash added to OPC) were degraded using similar protocols. Equilibrium solutions and solid materials were characterised for three degradation states for each paste. All samples are free of portlandite and the pH of the equilibrated cement solutions vary in the range 9.8-12.2. Three calcium silicate hydrate phases (C-S-H) were synthesised in order to compare the sorption properties of degraded cement pastes and of hydrate phases in similar pH conditions. In order to avoid precipitation processes, the operational solubility limit was evaluated before batch experiments. These solubility values vary significantly in the pH range [9-13] with a 2.4×10-7 mol L-1 minimum at pH close to 10.5. In batch sorption experiments, the distribution ratio Rd values are high: 3×104-1.5×105 mL g-1. The uptake of U(VI) increases when comparing the least and the most degraded cement pastes whereas the initial composition of cement has relatively insensitive effect. Sorption isotherms, expressed as a log[U(VI)solid]/log [U(VI)solution] plots are linear. A slope of 1 is calculated indicating the predominance of sorption processes. As sorption and desorption values are close, the uptake mechanism seems reversible. The Rd values measured in C-S-H suspensions are in good agreement with Rd values of degraded cement pastes, and C-S-H materials could be one of the cementitious phases which control U(VI) uptake in cement pastes.
© 2004 Oldenbourg Wissenschaftsverlag GmbH
Articles in the same Issue
- 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
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- 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
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- Scanning transmission X-ray microscopy as a speciation tool for natural organic molecules
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- 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
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- 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
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Articles in the same Issue
- 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