Diffusion of Uranium in Compacted Bentonites in the Reducing Condition with Corrosion Products of Iron

1995 ◽  
Vol 412 ◽  
Author(s):  
Kazuya Idemitsu ◽  
Y. Tachi ◽  
H. Furuya ◽  
Y. Inagaki ◽  
T. Arima
Keyword(s):  
Carbon Steel ◽  
Pore Water ◽  
Diffusion Coefficients ◽  
Corrosion Products ◽  
Redox Conditions ◽  
High Level Waste ◽  
Dry Density ◽  
Apparent Diffusion Coefficients ◽  
Reducing Conditions ◽  
Apparent Diffusion

AbstractIn high-level waste repository, a carbon steel overpack will be corroded after closure. This will create a reducing environment in the vicinity of the repository. Reducing conditions are expected to retard the migration of redox-sensitive radionuclides such as uranium.The apparent diffusion coefficients of uranium were measured in compacted bentonites (Kunigel VI® and Kunipia F®, JAPAN) in contact with carbon steel and its corrosion products under reducing conditions or without carbon steel under oxidizing conditions for comparison. The apparent diffusion coefficients measured were 10-12 to 10-14 m2/s under oxidizing conditions and 10-13 to 10-14 m2/s under reducing conditions. There were significant effects of redox conditions, dry density (0.8 to 2.0 g/cm3) and montmorillonite contents (60% for Kunigel VI or 100% for Kunipia F) on the apparent diffusion coefficients. The sorption of uranium on corrosion products of iron was smaller than that on montmorillonite. Montmorillonite density could be a good index to explain density dependence of the diffusion coefficients under the reducing conditions. Uranium would diffuse in free pore water with diffusion coefficients greater than 10-13 m2/s in low density bentonites under both redox conditions because the diffusion coefficients depended on sorption coefficients. Since diffusion coefficients were independent of sorption coefficients in high density bentonites where free pore water is scarce, surface diffusion might occur with coefficients were of about 10-13 m2/s.

Diffusion of Cs and Sr in Compacted Bentonites Under Reducing Conditions and in the Presence of Corrosion Products of Iron

1997 ◽  
Vol 506 ◽  
Author(s):  
K. Idemitsu ◽  
Y Tachi ◽  
H. Furuya ◽  
Y. Inagaki ◽  
T. Arima
Keyword(s):  
Carbon Steel ◽  
Corrosion Product ◽  
Diffusion Coefficients ◽  
Corrosion Products ◽  
High Level Waste ◽  
Dry Density ◽  
Iron Corrosion ◽  
Apparent Diffusion Coefficients ◽  
Reducing Conditions ◽  
Apparent Diffusion

ABSTRACTIn high-level waste repositories, a carbon steel overpack will be corroded by consuming oxygen trapped in the repository after closure. Iron corrosion products are expected to interfere with migration of radionuclides by filling the pore in bentonite and sorbing radionuclides. In this study the apparent diffusion coefficients of cesium and strontium were measured in compacted Na-bentonites (Kunigel VI® and Kunipia F®, JAPAN) contacted with carbon steel and its corrosion products under reducing conditions or without carbon steel under oxidizing conditions for comparison. The apparent diffusion coefficients of cesium with and without corrosion product were 2.2 to 13 × 10−12 m2/s. The apparent diffusion coefficients of strontium with and without corrosion product were 3.1 to 25 × 10−12 m2/s. There were significant effects of dry density (0.8 to 2.0 g/cm3) and montmorillonite contents (50% for Kunigel V1 or 100% for Kunipia F). The presence of corrosion product decreased the apparent diffusion coefficients of Cs in both bentonites and that of Sr in Kunigel V1, especially at low dry density. This may be due to corrosion product filling the pore in the bentonite, decreasing the free pore size and density for diffusion.

Diffusion of Technetium in Compacted Bentonites in the Reducing Condition with Corrosion Products of Iron

1996 ◽  
Vol 465 ◽  
Author(s):  
Yuji Kuroda ◽  
K. Idemitsu ◽  
H. Furuya ◽  
Y. Inagaki ◽  
T. Arima
Keyword(s):  
Carbon Steel ◽  
Diffusion Coefficients ◽  
Corrosion Products ◽  
High Level Waste ◽  
Dry Density ◽  
Apparent Diffusion Coefficients ◽  
Reducing Conditions ◽  
Apparent Diffusion ◽  
Reducing Environment ◽  
High Level

ABSTRACTIn the vicinity of a high-level waste repository, corrosion of carbon steel overpacks will create a reducing environment. Reducing conditions are expected to retard the migration of redox-sensitive radionuclides such as technetium.The apparent diffusion coefficients of technetium were measured in compacted bentonites (Kunigel VI® and Kunipia F®, JAPAN) in contact with carbon steel and its corrosion products under reducing conditions or without carbon steel under oxidizing conditions for comparison. The apparent diffusion coefficients measured were 10-12 to 10-13 m2/s under oxidizing conditions and 10-12 to 10-13 m2/s under reducing conditions. There were significant effects of redox condition, dry density (0.2 to 2.3 g / cm3) and montmorillonite content (50% for Kunigel VI or 100% for Kunipia F) on the apparent diffusion coefficients. Montmorillonite density could be a good index to explain density dependence of the diffusion coefficients under both reducing and oxidizing conditions.

Effect of pH on Plutonium Migration Behavior in Compacted Bentonite

MRS Advances ◽  
2016 ◽  
Vol 1 (61) ◽  
pp. 4011-4017
Author(s):  
Ryo Hamada ◽  
Noriyuki Maeda ◽  
Kazuya Idemitsu ◽  
Yaohiro Inagaki ◽  
Tatsumi Arima ◽  
...  
Keyword(s):  
Pore Water ◽  
Diffusion Coefficients ◽  
High Level Waste ◽  
Migration Behavior ◽  
Effect Of Ph ◽  
Apparent Diffusion Coefficients ◽  
Compacted Bentonite ◽  
Ph Values ◽  
Apparent Diffusion ◽  
High Level

ABSTRACTIn disposing of high-level radioactive waste, the drop in pH in the repository as the iron overpack corrodes must be considered. Plutonium migration behavior may be affected by the pH of pore water in compacted bentonite barriers in high-level waste repositories. To examine the effect of pH on migration behavior, H-bentonite was prepared by treating Japanese Na-bentonite, Kunipia-F, with hydrochloric acid. Diffusion experiments were performed with mixtures of Na- and H-bentonites. The pH value in the pore water of the water-saturated bentonite mixtures decreased from 8 to 3 as the mixing ratio of H-bentonite increased. Diffusion experiments were carried out by using238Pu then apparent diffusion coefficients were determined from the plutonium distribution in the specimens. The apparent diffusion coefficients were on the order of 10-13to 10-12m2/s at pH values lower than 4, whereas they were less than 10-14m2/s at pH values higher than 6.5. These results indicate that plutonium diffused faster as Pu3+or PuO22+due to disproportionation at lower pH while plutonium could be retarded as Pu(OH)40by sorption on bentonite at higher pH.

Diffusion of Uranium in Compacted Bentonite in the Presence of Carbon Steel

1993 ◽  
Vol 333 ◽  
Author(s):  
K. Idemitsu ◽  
H. Furuya ◽  
Y. Tachi ◽  
Y. Inagaki
Keyword(s):  
Carbon Steel ◽  
Pore Water ◽  
Silica Sand ◽  
High Level Waste ◽  
Dry Density ◽  
Compacted Bentonite ◽  
Reducing Conditions ◽  
Order Of Magnitude ◽  
The Difference ◽  
High Level

ABSTRACTIn a high-level waste repository, a carbon steel overpack will be corroded by consuming oxygen trapped in the repository after closure. This will create a reducing environment in the vicinity of repository. Reducing conditions are expected to retard the migration of redox-sensitive radionuclides such as uranium.The apparent diffusivities of uranium were measured in compacted bentonite (Kunigel VI®, Japan) in contact with carbon steel under reducing conditions or without carbon steel under oxidizing conditions for comparison. The apparent diffusivities of uranium were 3.5 × 10-14 to 1.1 × 10-13 m2/s under reducing conditions and 9.0 × 10-13 to 1.4 × 10-12 m2/s under oxidizing conditions. There was no significant effect of dry density (1.6 to 1.8 g/cm3) and silica sand (0 or 40%) on the apparent diffusivities.Since the bentonite pore water would be buffered at a pH between 8 and 9, uranium in the bentonite pore water would probably exist as a neutral hydroxide complex under reducing conditions and as an anioníc carbonate or hydroxide complex under oxidizing conditions. The anion exclusion theory cannot explain the difference of diffusivities between the two conditions. The uranium concentrations in bentonite under oxidizing conditions were one order of magnitude higher than those under the reducing conditions. The uranium concentration in the bentonite pore water under the reducing condition is estimated to be two orders of magnitude lower than that under the oxidizing conditions under the assumption of diffusion in porous media.

Hydraulic and Diffusive Properties of Clay-Based Backfill Material for a Low-and Intermediate-Level Waste Repository

1994 ◽  
Vol 353 ◽  
Author(s):  
W.J. Cho ◽  
J.O. Lee ◽  
P.S. Hahn ◽  
H.H. Park
Keyword(s):  
Diffusion Coefficients ◽  
Experimental Studies ◽  
Clay Content ◽  
Dry Density ◽  
Compacted Clay ◽  
Southeastern Part ◽  
Apparent Diffusion Coefficients ◽  
Crushed Granite ◽  
Apparent Diffusion ◽  
Water Saturated

AbstractThe results of experimental studies performed to determine the radionuclide diffusion coefficients in a compacted clay and the hydraulic conductivities of clay/crushed granite mixtures with various clay contents are presented. Clay used in the experiments is a natural clay from the southeastern part of Korea, and it contains mainly calcium bentonite. The hydraulic conductivities of clay/crushed granite mixtures decreased with increasing clay content. In case of clay content of 50 wt.%, they maintain the considerably lower values even at the dry density of 1.5 Mg/m3. The diffusion coefficients for 90Sr, 137Cs, 60Co and 125I in water saturated clay at a dry density of 1.4 Mg/m3 were measured at room temperature. The average apparent diffusion coefficients obtained are 4.5 × 10−12 m2/s, 9.0 ×10−13 m2/s, 3.4 × 10−13 m2/s and 6.7 × 10−11 m2/s for 90Sr, 137Cs, 60Co, and 125I, respectively.

Distribution Coefficients and Apparent Diffusion Coefficients of Cesium in Compacted Bentonites

1999 ◽  
Vol 556 ◽  
Author(s):  
Akiko Okamoto ◽  
Kazuya Idemitsu ◽  
Hirotaka Furuya ◽  
Yaohiro Inagaki ◽  
Tatsumi Arima
Keyword(s):  
Diffusion Coefficients ◽  
Distribution Coefficients ◽  
Dry Density ◽  
Apparent Diffusion Coefficients ◽  
Compacted Bentonite ◽  
Apparent Diffusion ◽  
Tracer Solution ◽  
Cesium Concentration ◽  
Penetration Profile ◽  
Very High

AbstractDistribution coefficients and apparent diffusion coefficients of cesium in some compacted bentonites were determined by the penetration profile method. Cylindrical compacted bentonites with the dry density of 0.8 to 1.6 Mg/m3 were contacted with tracer solutions containing 1000, 100 or 10 ppm of cesium. The apparent diffusion coefficients were obtained from the concentration profiles of cesium in compacted bentonites. The distribution coefficients were obtained concurrently by dividing the intercepts of the profiles by the concentration of the tracer solution. The apparent diffusion coefficients of cesium in compacted bentonite were obtained in the range of 0.42 to 9.6· 10−12 m2/s. The apparent diffusion coefficients in the compacted bentonite contacted with three different concentrations of cesium tended to decrease with increasing dry density of the specimen; but, they had no dependence on cesium concentration within a factor of 3 at the same dry density. The distribution coefficient of cesium for the specimens contacted with three different concentrations of cesium were obtained in the range of 0.3 to 90 L/kg and had little dependence on dry density. The distribution coefficients obtained in the compacted bentonites were dependent on pH of the solution rather than concentration of cesium. These distribution coefficients obtained in the compacted bentonites were 10 to 1000 times smaller than those obtained by batch experiments. The data suggest that not all sorption sites for cesium are available in highly compacted bentonite. It is necessary to consider surface diffusion as a significant migration mechanism of cesium through the compacted bentonites at very high pH condition such as 12.

The Dependence of the Diffusion Coefficients of 3H and Cs on Grain Size in Compacted Montmorillonite

1997 ◽  
Vol 506 ◽  
Author(s):  
Mamoru Nakajima ◽  
Tamotsu Kozaki ◽  
Hiroyasu Kato ◽  
Seichi Sato ◽  
Hiroshi Ohashi
Keyword(s):  
Grain Size ◽  
Diffusion Coefficients ◽  
Dry Density ◽  
Formation Factor ◽  
Apparent Diffusion Coefficients ◽  
Compacted Bentonite ◽  
Buffer Material ◽  
Apparent Diffusion ◽  
Different Grain Size ◽  
High Level

ABSTRACTCompacted bentonite is a candidate buffer material in geological disposal of high-level radioactive waste. The transport of radionuclides in compacted bentonite is dominated by diffusion, because of its very low permeability. In this study, we focused on the grain size of clay mineral, which is considered to be closely related to the formation factor in the pore water diffusion model[1,2]. The apparent diffusion coefficients (Da) of HTO and cesium ions in compacted clays were determined using montmorillonite samples with different grain size and dry density, and the effect of the grain size on diffusion behavior was discussed.

Effect of Carbonate on the Migration Behavior of Lanthanides in Compacted Bentonite

MRS Advances ◽  
2018 ◽  
Vol 3 (21) ◽  
pp. 1155-1160 ◽  
Author(s):  
Kazuya Idemitsu ◽  
Kazuyuki Fujii ◽  
Noriyuki Maeda ◽  
Yuki Kakoi ◽  
Noriya Okubo ◽  
...  
Keyword(s):  
Diffusion Coefficient ◽  
Atomic Number ◽  
Diffusion Coefficients ◽  
Chemical Species ◽  
Dry Density ◽  
Migration Behavior ◽  
Bicarbonate Concentration ◽  
Apparent Diffusion Coefficients ◽  
Carbonate Ion ◽  
Apparent Diffusion

ABSTRACTThe apparent diffusion coefficients of La, Nd, Eu, Dy, Er, and Lu in compacted bentonites were investigated at various bicarbonate concentrations. The apparent diffusion coefficients of these lanthanides tended to decrease with increasing dry density. At bicarbonate concentrations below 0.25 M, lanthanum had the largest diffusion coefficient (ca. 10-13 m2/s) at 1.0 Mg/m3, and the diffusion coefficient decreased with increasing atomic number. On the other hand, at bicarbonate concentrations above 0.25 M, lutetium had the largest diffusion coefficient, and the diffusion coefficient decreased with decreasing atomic number. In particular, lanthanum and neodymium had diffusion coefficients below 10-14 m2/s, even at 1.0 Mg/m3. The diffusion coefficient of europium was around 10-13 m2/s at 1.0 Mg/m3 and was influenced less by the bicarbonate concentration. The diffusion coefficient of lutetium increased from 2 × 10-14 to 10-12 m2/s as the bicarbonate concentration was increased to 1.0 M. The concentration of carbonate ion in the pore water of bentonite is estimated to be much lower than that in solutions in contact with bentonite from the viewpoints of solubility and chemical species of lanthanides.

Migration Behavior of Ferrous Ions in Compacted Bentonite Under Reducing Conditions Using Electromigration

2004 ◽  
Vol 824 ◽  
Author(s):  
Kazuya Idemitsu ◽  
Xiaobin Xia ◽  
Yoshiro Kikuchi ◽  
Yaohiro Inagaki ◽  
Tatsumi Arima
Keyword(s):  
Carbon Steel ◽  
Corrosion Rate ◽  
Electrical Potential ◽  
Infiltration Rate ◽  
Corrosion Products ◽  
Ferrous Ion ◽  
High Level Waste ◽  
Dry Density ◽  
Compacted Bentonite ◽  
Buffer Material

AbstractCarbon steel is one of the candidate overpack materials for high-level waste disposal and is expected to assure complete containment of vitrified waste glass during an initial period of 1000 years in Japan. The lifetime of the carbon steel overpack will depend on its corrosion rate. The corrosion rate of carbon steel is reduced by the presence of buffer material such as bentonite. Buffer material will delay the supply of corrosive materials and discharge of corrosion products through it. Carbon steeloverpack will be corroded by consuming oxygen introduced by repository construction after closure of repository and then will keep the reducing environment in the vicinity of repository. Therefore, it is important to study the migration of iron corrosion products through the buffer material because it may affect the corrosion rate of overpack, migration of redox-sensitive radionuclides, and the properties of the buffer material. Electromigration experiments have been carried out with source of iron ions supplied byanode corrosion of iron coupon in compacted bentonite. The carbon steel coupon was connected as the working electrode to the potentiostat and was held at a constant applied potential between - 200 to 1000 mV vs. Ag/AgCl electrode for 48 hours. Corrosion currents were 0.5 to 2mA initially and depended on the supplied electrical potential, then decreased to approximately 0.1 mA in a few hours. The final corrosion current was independent of supplied electrical potential. It is expected that iron ion could migrate as ferrous ion through interlayer of montmorillonite replacing exchangeable sodium ions in the interlayer. The rate-determining process of this experimental configuration could be infiltration rate of ferrousioninto bentonite. Infiltration rate of ferrous ion into bentonite was increasing with dry density of bentonite.

Effect of Carbonate on the Migration Behavior of Strontium in Compacted Bentonite

MRS Advances ◽  
2019 ◽  
Vol 4 (17-18) ◽  
pp. 1021-1027
Author(s):  
Kazuya Idemitsu ◽  
Ryota Yamada ◽  
Masayuki Hirakawa ◽  
Yuki Kakoi ◽  
Hajime Arimitsu ◽  
...  
Keyword(s):  
Diffusion Coefficients ◽  
Inductively Coupled Plasma ◽  
Acrylic Resin ◽  
Diffusion Profile ◽  
Dry Density ◽  
Migration Behavior ◽  
Inductively Coupled ◽  
Apparent Diffusion Coefficients ◽  
Apparent Diffusion ◽  
The Face

ABSTRACTThe apparent diffusion coefficients of strontium in compacted bentonites were investigated at various concentrations of NaHCO3. Purified sodium bentonite Kunipia-F® was compacted with a jig into cylindrical pellets 10 mm in diameter and 10 mm high with dry densities of 1.0 to 1.6 Mg/m3. Each bentonite pellet was inserted into an acrylic resin column and saturated with carbonated water containing 0.1 to 1.0 M NaHCO3 for more than 1 month. The face of the bentonite specimen was spiked with 5 μL of 1.0 M SrCl2 tracer solution. After a few weeks, the strontium diffusion profiles were measured by inductively coupled plasma-mass spectrometry. The apparent diffusion coefficients of strontium decreased slightly with increasing dry density. NaHCO3 concentrations of 0.5 M decreased the apparent diffusion coefficients of strontium by half at a dry density of 1.0 Mg/m3 and quarter at 1.6 Mg/m3. At a higher NaHCO3 concentration of 1.0 M, no strontium diffusion profile was observed, whereas white precipitate was observed on the face of the bentonite specimen where it was spiked with strontium. This white precipitate could be strontianite, which is strontium carbonate. Diffusion experiments using cesium were carried out for comparison, and the presence of carbonate had no effect on the apparent diffusion coefficient.

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