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 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 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.

Corrosion of Iron and Migration of Corrosion Products in Compacted Bentonite

1994 ◽  
Vol 353 ◽  
Author(s):  
T. Kozaki ◽  
Y. Imamura ◽  
J. Takada ◽  
S. Sato ◽  
H. Ohashi
Keyword(s):  
Diffusion Coefficients ◽  
Corrosion Products ◽  
Iron Foil ◽  
Iron Corrosion ◽  
Apparent Diffusion Coefficients ◽  
Corrosion Rates ◽  
Compacted Bentonite ◽  
Apparent Diffusion ◽  
And Migration ◽  
High Level

AbstractFor safety assessment of the geological disposal of the high level radioactive waste, it is necessary to study corrosion of the overpack materials and migration of the corrosion products in the compacted bentonite. In the present study, average corrosion rates of iron foil and apparent diffusion coefficients of the corrosion products were determined using a neutron- activated iron foil. The average corrosion rates were on the order of 10-6m/y, while apparent diffusion coefficients were in the range from 10-12 to 10-14m2/s. No tendency to decrease in the corrosion rates with increasing corrosion time was observed. This suggests that the iron foil corrodes under reducing condition. Asymmetric concentration profiles of iron corrosion products were obtained in some experiments. It can be considered that either cathodic or anodic reaction would dominantly occur on one side of the iron foil surfaces and that each reaction would change the pH in pore water of bentonite specimens adjacent to the iron foil surfaces.

Diffusion of Corrosion Products of Iron in Compacted Bentonite.

1992 ◽  
Vol 294 ◽  
Author(s):  
K. Idemitsu ◽  
H. Furuya ◽  
Y. Inagaki
Keyword(s):  
Carbon Steel ◽  
Corrosion Product ◽  
Hydrogen Generation ◽  
Ferric Hydroxide ◽  
Corrosion Products ◽  
Ferrous Ion ◽  
Silica Sand ◽  
High Level Waste ◽  
Buffer Material ◽  
The Difference

ABSTRACTCarbon steel is one of the candidate overpack materials for high-level waste disposal. The corrosion rate of carbon steel is reduced by the presence of buffer materials such as bentonite and seems to be affected by the diffusion of corrosive materials and corrosion products through the buffer material.The apparent diffusivities of corrosion product of iron were measured in some bentonite specimens in contact with carbon steel. The apparent diffusivities of iron were also measured without carbon steel for comparison. The apparent diffusivities of corrosion product were on the order of 10−12 m2/s and showed a tendency to decrease with increasing density of the bentonite specimen. There was no significant effect of silica sand on the apparent diffusivities. The apparent diffusivities of iron in the system without carbon steel were in the range of 10−14 m2/s and showed a tendency to increase with increasing silica sand content. The difference of the diffusivities between corrosion product and iron without carbon steel seems to be due to the difference of diffusing species. The color of the corrosion product was dark-green during contact with bentonite specimens and became red on exposure to air in a few minutes. Gas bubbles were also observed in the corrosion product. This suggests hydrogen generation during corrosion of the carbon steel. Thus the diffusing species seems to be in a reduced state, probably ferrous ion. On the other hand, the diffusing species of iron without carbon steel was probably a ferric hydroxide complex that was negatively charged. This suggests that ferrous ion could diffuse in the surface water adsorbed on bentonite, while ferric complex was excluded.

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.

Migration Behaviour of Lanthanides in Compacted Bentonite with Iron Corrosion Product Using Electrochemical Method

2012 ◽  
Vol 1475 ◽  
Author(s):  
Kazuya Idemitsu ◽  
Daisuke Akiyama ◽  
Yoshihiko Matsuki ◽  
Yusuke Irie ◽  
Yaohiro Inagaki ◽  
...  
Keyword(s):  
Carbon Steel ◽  
Dispersion Coefficient ◽  
Reference Electrode ◽  
High Level Waste ◽  
Dry Density ◽  
Migration Behavior ◽  
Iron Corrosion ◽  
Compacted Bentonite ◽  
Steel Coupon ◽  
Best Fit

ABSTRACTAfter the closure of a high-level waste repository, corrosion of the carbon steel overpack will occur. The corrosion products can then migrate into bentonite and affect the migration behavior of radionuclides in bentonite. Therefore, electrochemical experiments, with Fe2+ supplied by anodic corrosion of carbon steel, were carried out to study trivalent lanthanides in compacted bentonite. The interface between a carbon steel coupon and bentonite (dry density, 1.5 Mg/m3) was spiked with a tracer solution containing Nd(NO3)3, Eu(NO3)3, Dy(NO3)3, and Er(NO3)3. The carbon steel coupon was connected as the working electrode to a potentiostat and held at a constant potential between -550 and 0 mV (vs. Ag/AgCl reference electrode) for 7 days. A model using dispersion and electromigration could explain the measured profiles in the bentonite specimens. The best-fit electromigration velocity was related to the applied electric potential and was 1.0–3.8 nm/s for Nd, Eu, Dy, and Er ions. For these lanthanides, the best-fit dispersion coefficient was also related to the applied potential and was 0.8–1.6 μm2/s, and the dispersion length was calculated as 0.2 mm from the linear relationship between the dispersion coefficient and electromigration velocity. Finally, the apparent diffusion coefficient for these lanthanides was estimated as 0.6–0.9 μm2/s.

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.

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