Sorption and diffusion of organic acids through clayrock: Comparison with inorganic anions

Dagnelie, R.; Descostes, Michaël; Pointeau, Ingmar; Klein, J. C.; Grenut, B.; Radwan, J.; Lebeau, D.; Georgin, Dominique; Giffaut, Éric

doi:10.1016/j.jhydrol.2014.02.002

Cited by 16 publications

(15 citation statements)

References 49 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The values for K d and K d * are 3.8 L kg -1 and 0.089 L kg -1 respectively. These are still consistent with values previously obtained on COx samples by through-diffusion experiment, with K d~6 .2 L kg -1 measured by batch experiment and K d~0 .08 L kg -1 measured by through-diffusion (Dagnelie et al, 2014). The adsorption value (K d ) is more likely representative of total capacity of adsorption, as measured in batch or in-diffusion experiment.…”

Section: Transport and Behaviour Of Edtasupporting

confidence: 90%

“…Strikingly, it was not possible to adjust both liquid monitoring and solid profile for EDTA results, using only (D e , α) as parameters. We did not use a specific adsorption law for EDTA since the adsorption isotherm measured on COx clay is almost linear from 10 -7 up to 10 -2 mol L -1 (Dagnelie et al, 2014). The best fit obtained with two parameters (D e , α) displays a large underestimation of the decrease of the liquid concentration.…”

Section: Transport and Behaviour Of Edtamentioning

confidence: 99%

“…We chose to study a Callovo-Oxfordian (COx) clay rock, which is investigated by the French radioactive waste management agency (Andra, 2014;Gaucher et al, 2004) in the context of the underground retrievable nuclear waste repository project (Cigéo). Numerous data are available on this clay rock, including diffusion of cations (Melkior et al, 2007), diffusion of anions (Descostes et al, 2008;Savoye et al, 2012a), diffusion of organic co-contaminants (Dagnelie et al, 2014) and organic macromolecules (Durce et al, 2014). Most of these studies use standard diffusion cells at a centimetric scale.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Perturbation induced by EDTA on HDO, Br- and EuIII diffusion in a large-scale clay rock sample

Dagnelie

Arnoux

Radwan

et al. 2015

Applied Clay Science

Self Cite

View full text Add to dashboard Cite

Section: Transport and Behaviour Of Edtasupporting

confidence: 90%

Section: Transport and Behaviour Of Edtamentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Perturbation induced by EDTA on HDO, Br- and EuIII diffusion in a large-scale clay rock sample

Dagnelie

Arnoux

Radwan

et al. 2015

Applied Clay Science

Self Cite

View full text Add to dashboard Cite

“…Thus, the occurrence and potential interactions of natural chelating agents, i.e. (P)HCA, with radionuclides is of crucial importance for safety assessment of cementitious geological disposal facilities [ 6 , 11 , 12 ].…”

Section: Introductionmentioning

confidence: 99%

Adsorption of aliphatic polyhydroxy carboxylic acids on gibbsite: pH dependency and importance of adsorbate structure

Schneckenburger¹,

Riefstahl²,

Fischer

2018

Environ Sci Eur

View full text Add to dashboard Cite

BackgroundAliphatic (poly)hydroxy carboxylic acids [(P)HCA] occur in natural, e.g. soils, and in technical (waste disposal sites, nuclear waste repositories) compartments . Their distribution, mobility and chemical reactivity, e.g. complex formation with metal ions and radionuclides, depend, among others, on their adsorption onto mineral surfaces. Aluminium hydroxides, e.g. gibbsite [α-Al(OH)3], are common constituents of related solid materials and mimic the molecular surface properties of clay minerals. Thus, the study was pursued to characterize the adsorption of glycolic, threonic, tartaric, gluconic, and glucaric acids onto gibbsite over a wide pH and (P)HCA concentration range. To consider specific conditions occurring in radioactive wastes, adsorption applying an artificial cement pore water (pH 13.3) as solution phase was investigated additionally.ResultsThe sorption of gluconic acid at pH 4, 7, 9, and 12 was best described by the “two-site” Langmuir isotherm, combining “high affinity” sorption sites (adsorption affinity constants > 1 L mmol−1, adsorption capacities < 6.5 mmol kg−1) with “low affinity” sites ( < 0.1 L mmol−1, adsorption capacities ≥ 19 mmol kg−1). The total adsorption capacities at pH 9 and 12 were roughly tenfold of that at pH 4 and 7. The S-shaped pH sorption edge of gluconic acid was modelled applying a constant capacitance model, considering electrostatic interactions, hydrogen bonding, surface complex formation, and formation of solved polynuclear complexes between Al3+ ions and gluconic acid. A Pearson and Spearman rank correlation between (P)HCA molecular properties and adsorption parameters revealed the high importance of the size and the charge of the adsorbates.ConclusionsThe adsorption behaviour of (P)HCAs is best described by a combination of adsorption properties of carboxylic acids at acidic pH and of polyols at alkaline pH. Depending on the molecular properties of the adsorbates and on pH, electrostatic interactions, hydrogen bonding, and ternary surface complexation contribute in varying degrees to the adsorption process. Linear distribution coefficients Kd between 8.7 and 60.5 L kg−1 (1 mmol L−1 initial PHCA concentration) indicate a considerable mineral surface affinity at very high pH, thus lowering the PHCA fraction available for the complexation of metal ions including radionuclides in solution and their subsequent mobilization.

show abstract

“…The effect of the size of diffusing molecules on its diffusion coefficient in CallovoOxfordian Clay has also been discussed by Dagnelie et al [35]. For anions, a relation was shown between the anion size (expressed as 1/3 with the molecular mass) and the ratio of aqueous diffusion coefficients 0 / 0 HTO .…”

Section: Introductionmentioning

confidence: 86%

The Dependency of Diffusion Coefficients and Geometric Factor on the Size of the Diffusing Molecule: Observations for Different Clay-Based Materials

et al. 2017

View full text Add to dashboard Cite

In order to investigate in more detail the relation between the size of diffusing molecules and their diffusion coefficients (and geometric factors), diffusion experiments with gases of different size and tritiated water (HTO) have been performed on different clayey samples (Boom Clay, Eigenbilzen Sands, Opalinus Clay, Callovo-Oxfordian Clay, and bentonite with different dry densities). We observed that, for unreactive gases in clayey materials, the effective diffusion coefficient varies with the size of the diffusing molecule and this variation can be described by an exponential or a power law function. The variation of the geometric factor can also be described by an exponential function. The observed experimental relations can be used to estimate diffusion coefficients; by measuring experimentally in clay the effective diffusion coefficient of two unreactive dissolved gases with a different size, the diffusion coefficients of other dissolved gases (with a size in between the two measured gases) can be estimated by using the fitted exponential relationship.

show abstract

Sorption and diffusion of organic acids through clayrock: Comparison with inorganic anions

Cited by 16 publications

References 49 publications

Perturbation induced by EDTA on HDO, Br- and EuIII diffusion in a large-scale clay rock sample

Perturbation induced by EDTA on HDO, Br- and EuIII diffusion in a large-scale clay rock sample

Adsorption of aliphatic polyhydroxy carboxylic acids on gibbsite: pH dependency and importance of adsorbate structure

The Dependency of Diffusion Coefficients and Geometric Factor on the Size of the Diffusing Molecule: Observations for Different Clay-Based Materials

Contact Info

Product

Resources

About