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JAEA-Review-2010-065.pdf:15.99MB - 日本原子力研究開発機構

JAEA-Review-2010-065.pdf:15.99MB - 日本原子力研究開発機構

JAEA-Review-2010-065.pdf:15.99MB - 日本原子力研究開発機構

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Study on Stability of Cs·Sr Solvent Impregnate Resin<br />

against Gamma Irradiation<br />

H. Hoshi a) , T. Kikuchi a) , Y. Morita a) and T. Kimura b)<br />

a) Division of Fuels and Materials Engineering, NSED, <strong>JAEA</strong>,<br />

b) Division of Environment and Radiation Sciences, NSED, <strong>JAEA</strong><br />

Minimization of radioactive waste from reprocessing<br />

process of spent nuclear fuel is strongly desired. We have<br />

developed an advanced technology for separation of heat<br />

generating elements (Cs and Sr) from high level waste to<br />

optimize radioactive waste by its characteristics. Recently,<br />

some analogues of calix-crown or crown ether extractant<br />

were reported on specific selectivity for Cs or Sr,<br />

respectively 1,2) . In our previous study, prepared adsorbents<br />

indicated promising ability to separate Cs and Sr from other<br />

typical fission products dissolved in nitric acid solution;<br />

besides they maintained significant selectivity for Cs or Sr<br />

after gamma irradiation. Decreasing ratio of static<br />

adsorption capacity by irradiation was also estimated. In this<br />

work, gamma irradiation effect on dynamic adsorption<br />

capacity was examined for the conceptual designing.<br />

An extractant and a modifier were impregnated into<br />

porous silica, which is embedded styrene divinyl benzene<br />

polymer on the surface. These adsorbents contacting with<br />

nitric acid solution were exposed to gamma ray in a vial.<br />

The dynamic adsorption capacity was examined by using<br />

irradiated adsorbents. The irradiated adsorbent was packed<br />

in a glass column as slurry state. After the packed column<br />

was filled with 3 M HNO 3, a break through curve was<br />

obtained by feeding HNO 3 solution containing 10 mM Cs or<br />

Sr.<br />

Initial dynamic adsorption capacity was estimated in<br />

advance and was 70.2 mmol/L, which was obtained by the<br />

product of Cs concentration and the difference between the<br />

break through point and the dead volume. Figure 1 shows<br />

[Cs] / mM<br />

1-15<br />

10<br />

8<br />

6<br />

4<br />

2<br />

Dead<br />

volume<br />

0<br />

0 10 20 30 40 50 60<br />

Effluent volume / cm 3<br />

54.9 cm 3<br />

Fig. 1 Breakthrough curve of Cs adsorbent after gamma<br />

irradiation. Dose rate: 1.82 kGy/h; duration: 16 h;<br />

Dose: 29.1 kGy; soaked in 3 M HNO3. Column: i.d.<br />

10 mm × 100 mm height (bed height: 82 mm); flow<br />

rate: 1 cm 3 /min; mobile phase: 10 mM Cs-3 M HNO3. <strong>JAEA</strong>-<strong>Review</strong> <strong>2010</strong>-065<br />

the break through curve of Cs adsorbent, which was<br />

irradiated 29.1 kGy in 3 M HNO 3. The breakthrough point<br />

was estimated at 54.9 cm 3 by linear regression (dotted line).<br />

The dynamic adsorption capacity of irradiated adsorbent<br />

was 73.5 mmol/L, which was almost as same as initial one.<br />

This result indicated that this adsorbent has rather high<br />

stability against gamma irradiation.<br />

Figure 2 shows the break through curve of Sr adsorbent,<br />

which was irradiated 29.1 kGy in 3 M HNO 3. While initial<br />

dynamic adsorption capacity was 125 mmol/L, that of<br />

irradiated adsorbent was 87.1 mmol/L; the dynamic<br />

adsorption capacity decreased by around 30%. Thus, some<br />

refinement of process design will be required.<br />

It is concluded that Cs adsorbent maintained its dynamic<br />

adsorption capacity and Sr adsorbent kept 70% of initial<br />

capacity. Decreasing ratio of dynamic adsorption capacity<br />

by irradiation can be estimated from these results. It<br />

contributes significantly for the conceptual design of<br />

separation plant.<br />

Present study is the result of “Development of separation<br />

technology of transuranium elements and fission products<br />

by using new extractants and adsorbents” entrusted to <strong>JAEA</strong><br />

by the Ministry of Education, Culture, Sports, Science and<br />

Technology of Japan (MEXT). We are very grateful to<br />

Mr. Yamagata for his valuable cooperation in this study.<br />

References<br />

1) P. V. Bonnesen et al., Solve. Extr. Ion Exch. 18 (2000)<br />

1079.<br />

2) J. F. Dozol et al., EUR 19605EN, 2000.<br />

[Sr] / mM<br />

- 19 -<br />

10<br />

8<br />

6<br />

4<br />

2<br />

Dead<br />

volume<br />

62.3 cm 3<br />

0<br />

0 10 20 30 40 50 60 70 80<br />

Effluent volume / cm 3<br />

Fig. 2 Breakthrough curve of Sr adsorbent after gamma<br />

irradiation. Dose rate: 1.82 kGy/h; duration: 16 h;<br />

Dose: 29.1 kGy; soaked in 3 M HNO3. Column i.d.:<br />

10 mm × 100 mm height (bed height: 80 mm); flow<br />

rate: 1 cm 3 /min; aq. phase: 10 mM Sr-3 M HNO3.

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