Activation energy of diffusivities for deuterated water in compacted sodium-bentonite; Through-diffusion experiment and molecular dynamics simulation

Suzuki, Satoru; Sato, Haruo; Ishidera, Takamitsu; Fujii, Naoki*; Kawamura, Katsuyuki*

JNC TN8400 2001-031, 44 Pages, 2002/05

JNC-TN8400-2001-031.pdf:1.58MB

In order to quantify effect of temperature on diffusivity of deuterated water (HDO) in compacted sodium-bentonite, through-diffusion experiments were conducted at elevated tempemture from 298 to 333 K. Kunipia F (Na-montmorillonite content 98 wt. %; Kunimine Industly Co.) was compacted to a dry density of 0.9 and l.35 Mg/m. Since smectite flakes were perpendicularly oriented to a direction of compaction, anisotropy of diffusivity was investigated parallel and normal to the preferred orientation of smectite. Effective diffusion coeficient D of HDO was larger for a diffusional direction parallel to the preferred orientation than normal to that for both dry densities. These results well agreed to the previously reported ones for tritiated water. Activation energies of D in compacted bentonite increased with increasing dry density in the range of 19 - 25 kJ/mol which was slightly larger than that in bulk water (18 kJ/mol). This relationship can be considered to be due to both the pore structure development and high activation energy of water (18-23 kJ/mol) in the vicinity of smectite surface (within 2 nm) on the basis of molecular dynamics simulations.