Conceptual Modeling of the Humic Colloid-Borne Americium(III) Migration by a Kinetic Approach

Schuessler, Wolfram; Artinger, Robert; Kienzler, Bernhard; Kim, Jae-Il

doi:10.1021/es991246a

Cited by 44 publications

(34 citation statements)

References 28 publications

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“…Its relatively large portion in the strong hydrophobic fraction (SPE cartridge) is consistent with the association of 241 Am with NOM in other studies (Artinger et al, 1998;Schuessler et al, 2000;Cooper et al, 1995, to name a few). Our sample somewhat contrasts the findings of Cooper et al (1995), because their chromatographic separation suggested that 241 Am was associated with the smaller-sized NOM.…”

Section: Americium-241supporting

confidence: 88%

“…Our sample somewhat contrasts the findings of Cooper et al (1995), because their chromatographic separation suggested that 241 Am was associated with the smaller-sized NOM. The work at the Gorleben site (Artinger et al, 1998;Schuessler et al, 2000) is particularly significant, because the authors deal with the kinetics of association/dissociation of Am with NOM. Their experiments extended over several thousands of hours (months), and they obtained both kinetic and equilibrium constants, with more than one binding site.…”

Section: Americium-241mentioning

confidence: 99%

See 1 more Smart Citation

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

Mankarios

2004

Journal of Environmental Radioactivity

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Section: Americium-241supporting

confidence: 88%

Section: Americium-241mentioning

confidence: 99%

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

Mankarios

2004

Journal of Environmental Radioactivity

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“…The additivity of the models for mixed illite/NOM systems will now be tested. However, the two models rely on equilibrium conditions being present in the experimental systems, and radionuclide interactions in quasi-natural systems containing dissolved NOM are known to exhibit slow kinetic rates (e.g., [30][31][32]). Thus, it must be verified whether the measured Eu solid-liquid distribution is truly for equilibrium conditions.…”

Section: Sorption Of Europium In Combined Illite/nom (Ternary) Systemsmentioning

confidence: 99%

Influence of Boom Clay organic matter on the adsorption of Eu³⁺by illite – geochemical modelling using the component additivity approach

Bruggeman

Liu

Maes³

2010

Ract

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Europium / Sorption modelling / Natural organic matter / Boom Clay / Complexation / Component additivitySummary. The solid-liquid distribution of europium (Eu) between an adsorptive surface and a solution phase containing a competitive colloid is the result of a delicate balance between several individual chemical reactions. In this study, adsorption isotherms of Eu in presence of dissolved Boom Clay natural organic matter were experimentally determined under conditions relevant for a geological repository (trace Eu concentrations, anoxic conditions, ∼ 0.014 mol l −1 NaHCO 3 background electrolyte). It was found that both the concentration and size distribution (or operational cut-off used to discriminate between "mobile" and "immobile" colloids) of natural organic matter has a strong influence on the observed solid-liquid distribution.The experimental data were subsequently modelled using a component additive approach with two well-established sorption/interaction models: the 2 SPNE SC/CE model for describing Eu adsorption on illite, and Humic Ion-Binding Model VI for describing Eu complexation to natural organic matter. Model parameters were gathered from dedicated measurements in batch systems containing only Eu and the interacting phase under study, under similar conditions as in the ternary isotherm experiments. Mutual interactions between illite and natural organic matter were studied and quantified. Under the experimental conditions of this study, it was found that these interactions were only of minor importance.The two models were subsequently combined to blind predict the Eu solid-liquid distribution in the ternary batch experiments. Within an error margin of 0.5 log K d units, the additivity approach succeeded well in predicting Eu uptake in all experimental systems studied. A sensitivity analysis was performed to select the most important model parameters influencing the Eu uptake, and the robustness of the model. This study has shown that the component additivity approach for describing and predicting uptake of trivalent lanthanides/actinides under Boom Clay conditions, is promising, and may help in unraveling the complex behaviour of these radionuclides witnessed in migration experiments.

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“…Another factor that could affect the sorption of the radionuclides concerned and of weighable amounts of uranium and stable Eu is formation of their hydrolyzed species at high pH typical of Yenisei river water (pH > 7.5) [21,22]. As a result, radionuclide-containing multicomponent polymeric hydroxo complexes…”

Section: Sorption Kinetics Of 241 Am and 242 Pu Tracers And Weighablementioning

confidence: 99%

Model Assessment of the Migration Capability of Transuranium Radionuclides (241Am and Pu Isotopes) and 152Eu in the System Bottom Sediments-Yenisei River Water by Chemical Fractionation Technique

et al. 2005

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Sorption of radiotracers 241 Am and 242 Pu and weighable amounts of uranium and stable Eu on bottom sediments in the simulated system bottom sediments3Yenisei river water was studied. At a contact time of 40 min these metals are completely sorbed on the bottom sediments, presumably via association with organomineral complexes and hydrated gels. Along with sorption, these metals can form soluble complexes and stable colloids (pseudocolloids). The distribution factors of 241 Am and 242 Pu, and stable Eu in the simulated system between bottom sediments and liquid phases were calculated from the results of sorption experiments. The introduced 241 Am and 152 Eu initially present in radioactively contaminated bottom sediments of the Yenisei river show similar pattern of distribution over differently mobile fractions. The distribution of weighable amounts of stable Eu significantly differs from that of initially present 152 Eu and tracer 241 Am due to decelerated sorption of stable Eu and its considerably higher concentration. A significant part of 242 Pu, 241 Am, and 152 Eu is associated with mobile fractions of bottom sediments, which, under certain environmental conditions, can pass into river water as migrating species.The long-term operation of the Krasnoyarsk Mining and Chemical Combine (MCC) (Minatom of Russian Federation) gives rise to radioactive contamination of adjacent territories of the Krasnoyarsk krai. A great quantity of radionuclides ( 137 Cs, 60 Co, 152 Eu, transuranium elements) was released into the environment [1,2].The bottom sediments of the Yenisei river are efficient sorbents for radionuclides. Therefore, the major fraction of radionuclides released from MCC was accumulated in the bottom sediments in the vicinity of the discharge point. However, it is known that, under certain environmental conditions, radionuclides initially accumulated in the bottom sediments can transform to mobile species and enter the biogeochemical migration cycles [3,4]. The migration capability of radionuclides in the system bottom sediment3aqueous phase mainly depends on the sorption rate of radionuclides and sorption power of bottom sediments for radionuclides.Extensive data are available on the distribution of radionuclides and stable chemical elements over differently mobile fractions of bottom sediments, including data for Krasnoyarsk krai. The problem of migration of radionuclides in these systems was also analyzed [538]. In this study, the radionuclide speciation in bottom sediments was analyzed by an improved chemical fractionation technique. This technique allows more reliable determination of distribution of radionuclides and stable chemical elements over differently mobile fractions and better characterization of the occurrence forms of radionuclides in the bottom sediments.The aim of this study was to assess the migration capability of 241 Am, plutonium isotopes, and 152 Eu in the simulated system bottom sediments3Yenisei river water using a chemical fractionation technique. EXPERIMENTALSampling and character...

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Conceptual Modeling of the Humic Colloid-Borne Americium(III) Migration by a Kinetic Approach

Cited by 44 publications

References 28 publications

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

Influence of Boom Clay organic matter on the adsorption of Eu³⁺by illite – geochemical modelling using the component additivity approach

Model Assessment of the Migration Capability of Transuranium Radionuclides (241Am and Pu Isotopes) and 152Eu in the System Bottom Sediments-Yenisei River Water by Chemical Fractionation Technique

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Conceptual Modeling of the Humic Colloid-Borne Americium(III) Migration by a Kinetic Approach

Cited by 44 publications

References 28 publications

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

Pre-assessment of the speciation of 60Co, 125Sb, 137Cs and 241Am in a contaminated aquifer

Influence of Boom Clay organic matter on the adsorption of Eu3+by illite – geochemical modelling using the component additivity approach

Model Assessment of the Migration Capability of Transuranium Radionuclides (241Am and Pu Isotopes) and 152Eu in the System Bottom Sediments-Yenisei River Water by Chemical Fractionation Technique

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Influence of Boom Clay organic matter on the adsorption of Eu³⁺by illite – geochemical modelling using the component additivity approach