Self-diffusion coefficients and structure of the trivalent transplutonium ion curium and gadolinium in aqueous solution

Latrous, H.; Oliver, J. H.

doi:10.1007/bf02038345

Cited by 12 publications

(6 citation statements)

References 18 publications

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“…The observed D values are of the order of 10 –6 cm 2 /s. These values are similar to the experimental observations . The D values show a decreasing trend with an increase in salt concentration.…”

Section: Resultssupporting

confidence: 90%

“…For DCHCE, the highest value of D is seen as ∼10 × 10 –6 cm 2 /s (at ρ s = 1.25 mol/nm 2 and C s = 0.05 M) and the lowest value of D is seen as 3 × 10 –6 cm 2 /s (at ρ s = 1.65 mol/nm 2 and C s = 0.5 M). It should be noted that the self-diffusion coefficient of Gd 3+ ion in bulk water is 6 × 10 –6 cm 2 /s . The D values observed in our simulation study are close to that of the bulk water at lower salt concentrations.…”

Section: Resultssupporting

confidence: 75%

“…These values are similar to the experimental observations. 44 The D values show a decreasing trend with an increase in salt concentration. For DCHCE, the highest value of D is seen as ∼10 × 10 −6 cm 2 /s (at ρ s = 1.25 mol/nm 2 and C s = 0.05 M) and the lowest value of D is seen as 3 × 10 −6 cm 2 /s (at ρ s = 1.65 mol/nm 2 and C s = 0.5 M).…”

Section: Experimental Isothermmentioning

confidence: 94%

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Adsorption of Gadolinium (Gd³⁺) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

et al. 2019

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All atom molecular dynamics simulations and experiments were performed to understand the adsorption behavior of gadolinium (Gd 3+ ) ion on the crown ethers grafted polystyrene (PS) surface. Two different types of crown ethers, viz., dibenzo crown ether (DBCE) and dicyclo hexano crown ether (DCHCE), were grafted separately on the PS surface to understand the adsorption behavior. We investigate the roles of Gd 3+ ion concentration and grafting density (ρ s ) of the crown ether on the adsorption behavior of Gd 3+ ion on the PS surface. The adsorption of Gd 3+ shows an increasing trend with increasing salt concentration, for all cases of crown ether grafting densities. The adsorption behavior follows the Langmuir isotherm model. The maximum amount of Gd 3+ ion adsorption was observed to be 1.83 mg/g for DBCE and 2.02 mg/g for DCHCE at ρ s = 2.07 mol/nm 2 . The maximum amount of Gd 3+ ion adsorption on DBCE coated PS beads, in batch experiments, was found to be 1.76 mg/g, which is in good agreement with the theoretical results. The increase in ρ s from 0.25 to 2.07 mol/nm 2 shows an increase in the q max value by ∼422% and 329% for DBCE and DCHCE, respectively. The optimum value of the crown ether grafting density is found to be 1.25 mol/nm 2 , beyond which the q max saturates. We further investigate the dynamics of the Gd 3+ ion by evaluating the diffusion coefficient (D) and mean residence time (τ). It was found that D decreases with increasing salt concentration for both DBCE and DCHCE. On the contrary, as expected, the τ value of Gd 3+ increases with an increase in salt concentration. Overall, a 3-fold increase in τ was seen with increasing salt concentration. The potential of mean force analysis using umbrella sampling reveals favorable binding energy for higher grafting density of DCHCE compared to that of DBCE.

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Section: Resultssupporting

confidence: 90%

Section: Resultssupporting

confidence: 75%

Section: Experimental Isothermmentioning

confidence: 94%

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Adsorption of Gadolinium (Gd³⁺) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

et al. 2019

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“…Table 3 lists radionuclide-specific transport properties. The molecular diffusion coefficient in bulk water for the radionuclides of interest can be calculated using the Stokes-Einstein law [75] or determined experimentally [76][77][78][79]. During the simulation, an effective diffusion coefficient is dynamically calculated to account for temperature effects and the impacts of salinity on viscosity according to the Stokes-Einstein equation [75].…”

Section: Processes and Parametersmentioning

confidence: 99%

“…Oxidation state at reducing Eh and pH between 7 and 9 2. Diffusion coefficient in bulk water at 25 • C[76][77][78][79] 3. Pessimistic K d -values from[81] Maximum solubility for granitic bedrock chemistries[11].…”

mentioning

confidence: 99%

Post-Closure Safety Analysis of Nuclear Waste Disposal in Deep Vertical Boreholes

Finsterle¹,

Muller

Grimsich

et al. 2021

Energies

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Isolation of spent nuclear fuel assemblies in deep vertical boreholes is analyzed. The main safety features of the borehole concept are related to the repository’s great depth, implying (a) long migration distances and correspondingly long travel times, allowing radionuclides to decay, (b) separation of the repository from the dynamic hydrological cycle near the land surface, (c) stable geological and hydrogeological conditions, and (d) a geochemically reducing environment. An integrated simulation model of the engineered and natural barrier systems has been developed to examine multiple scenarios of the release of radionuclides from the waste canisters, the transport through a fractured porous host rock, and the extraction of potentially contaminated drinking water from an aquifer. These generic simulations include thermal effects from both the natural geothermal gradient and the heat-generating waste, the influence of topography on regional groundwater flow, moderated by salinity stratification at depth, and the role of borehole sealing. The impact of these processes on the transport of select radionuclides is studied, which include long-lived, soluble, sorbing or highly mobile isotopes along with a decay chain of safety-relevant actinide metals. The generic analyses suggest that a deep vertical borehole repository has the potential to be a safe option for the disposal of certain waste streams, with the depth itself and the stable hydrogeological environment encountered in the emplacement zone providing inherent long-term isolation, which allows for reduced reliance on a complex engineered barrier system.

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Further insights in the ability of classical nonadditive potentials to model actinide ion–water interactions

et al. 2012

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Pursuing our efforts on the development of accurate classical models to simulate radionuclides in complex environments (Réal et al., J. Phys. Chem. A 2010, 114, 15913; Trumm et al. J. Chem. Phys. 2012, 136, 044509), this article places a large emphasis on the discussion of the influence of models/parameters uncertainties on the computed structural, dynamical, and temporal properties. Two actinide test cases, trivalent curium and tetravalent thorium, have been studied with three different potential energy functions, which allow us to account for the polarization and charge-transfer effects occurring in hydrated actinide ion systems. The first type of models considers only an additive energy term for modeling ion/water charge-transfer effects, whereas the other two treat cooperative charge-transfer interactions with two different analytical expressions. Model parameters are assigned to reproduce high-level ab initio data concerning only hydrated ion species in gas phase. For the two types of cooperative charge-transfer models, we define two sets of parameters allowing or not to cancel out possible errors inherent to the force field used to model water/water interactions at the ion vicinity. We define thus five different models to characterize the solvation of each ion. For both ions, our cooperative charge-transfer models lead to close results in terms of structure in solution: the coordination number is included within 8 and 9, and the mean ion/water oxygen distances are 2.45 and 2.49 Å, respectively, for Th(IV) and Cm(III).

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Self-diffusion coefficients and structure of the trivalent transplutonium ion curium and gadolinium in aqueous solution

Cited by 12 publications

References 18 publications

Adsorption of Gadolinium (Gd³⁺) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

Adsorption of Gadolinium (Gd³⁺) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

Post-Closure Safety Analysis of Nuclear Waste Disposal in Deep Vertical Boreholes

Further insights in the ability of classical nonadditive potentials to model actinide ion–water interactions

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Self-diffusion coefficients and structure of the trivalent transplutonium ion curium and gadolinium in aqueous solution

Cited by 12 publications

References 18 publications

Adsorption of Gadolinium (Gd3+) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

Adsorption of Gadolinium (Gd3+) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

Post-Closure Safety Analysis of Nuclear Waste Disposal in Deep Vertical Boreholes

Further insights in the ability of classical nonadditive potentials to model actinide ion–water interactions

Contact Info

Product

Resources

About

Adsorption of Gadolinium (Gd³⁺) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments

Adsorption of Gadolinium (Gd³⁺) Ions on the Dibenzo Crown Ether (DBCE) and Dicyclo Hexano Crown Ether (DCHCE) Grafted on the Polystyrene Surface: Insights from All Atom Molecular Dynamics Simulations and Experiments