Comparison of sorption coefficients between powder and intact solid phase: Case study with
133
Cs and
87
Sr on pumice tuff
*Mohammad Rajib
1
, Chiaki T. Oguchi
2
1.Graduate School of Science and Engineering, Saitama University/ Bangladesh Atomic Energy
Commission, 2.Department of Civil and Environmental Engineering, Saitama University
Adsorption experiment was carried out with both powdered and block pumice tuff to compare the
distribution coefficient (K
d
) values of stable cesium (
133
Cs) and strontium (
87
Sr) under variety of
geochemical conditions. The main objective was to infer the K
d
difference in laboratory and field
condition. Cs and Sr were selected as two important nuclides from low and intermediate lever
radioactive waste, and pumice tuff as one of the host rocks of such waste repositories. Pumice tuff
blocks were prepared for this study expecting that the block sample is nearly the ‘natural
condition’, like what is found in the field- compact with intact pores. Considering minimum
dependency of ionic strength, initial nuclide concentration and pH, 10
-4
mol/l Cs and Sr
concentration was selected as initial experimental concentration (Rajib et al., 2015, 2016) where
4, 8 and 12 were chosen as low, neutral and high pH conditions. Since ionic strength significantly
influences K
d
at less than 1.0 mol/l on pumice tuff (Rajib et al., 2011, 2016), relatively high
ionic strength of 1.0 and 3.0 mol/l was adopted. To keep the effect of particle size at minimum,
homogenous grain size of 150-300 μm was used for the powdered materials, whereas blocks were
prepared at an equal size of 1 cm
3
. Conventional batch technique was carried out with a
solid-solution ratio of 1:10. However, as the ratio cannot be kept fixed for block samples (the
weight varied from 1.090 to 1.456 g), adjustment to 1:10 ratio was necessary to recalculate K
d
values. After reaching equilibrium pH at the contact time of 14 weeks, Cs and Sr concentrations
were measured by ICP-MS, and the K
d
values were determined considering the natural dissolution of
Cs and Sr during aging period (Rajib et al., 2015). Pumice tuff samples were collected from below
50-100 m at subsurface where water-rock interaction occurred and a redox zone has been formed.
Hence, both fresh and oxidized pumice tuffs were possible to use to observe any oxidation effect.
To investigate surface area properties of pumice tuff, mercury intrusion porosimetry (MIP) and
observation through scanning electron microscope (SEM) was conducted.
The results show that K
d
values for block samples are considerably lower than powdered samples for
both Cs and Sr. Almost all the samples showed similar tendency with the average lower values of
8.79% for Cs and 4.94% for Sr in block samples of fresh tuff. In oxidized tuff, block samples
showed 14.58% and 13.65% lower values for Cs and Sr, respectively. The lower K
d
values on block
samples might be due to the use of lower surface area as sorption sites since many closed pores
exist in intact solid which cannot be accessed. The destruction of smaller pores in oxidized tuff
due to oxidation phenomena might be the cause of higher reducing K
d
values. However, use of pumice
tuff blocks for comparable batch adsorption experiment is possible due to its highly porous nature
where much amount of surface area can be accessed. The K
d
difference between block and powder
samples is expected to be caused mainly by the effect of diffusion, taking very long equilibrium
period, and the physical and mechanical properties of pores and fractures during experiment.
References:
1. Rajib, M., Kobayashi, T. Oguchi C. T. and Sasaki T. (2016), Journal of Geoscience and
Environment Protection, 4.
2. Rajib, M., Oguchi C. T., Sasaki T. and Kobayashi, T. (2015), Geochemical Journal, 49(5),
539-548.
3. Rajib, M., Sasaki, T., Kobayashi, T., Myaguchi, Y., Takagi, I. and Moriyama, H. (2011),
HCG25-13 Japan Geoscience Union Meeting 2016
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