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Migration Behavior of Plutonium in Compacted Bentonite Under Reducing Condition Using Electromigration

Published online by Cambridge University Press:  19 October 2011

Kazuya Idemitsu ,
Yosuke Yamasaki ,
Syeda Afsarun Nessa ,
Yaohiro Inagaki ,
Tatsumi Arima ,
Toshiaki Mitsugashira ,
Mitsuo Hara  and
Yoshimitsu Suzuki
Kazuya Idemitsu
Affiliation:
[email protected], Kyushu university, Applied Quantum Physics and Nuclear Engineering, 744 Motooka, Nishi-ku, Fukuoka, 812-0395, Japan, +81928023492, +81928023501
Yosuke Yamasaki
Affiliation:
[email protected], Kyushu university, Fukuoka, 819-0395, Japan
Syeda Afsarun Nessa
Affiliation:
[email protected], Kyushu university, Fukuoka, 819-0395, Japan
Yaohiro Inagaki
Affiliation:
[email protected], Kyushu university, Fukuoka, 819-0395, Japan
Tatsumi Arima
Affiliation:
[email protected], Kyushu university, Fukuoka, 819-0395, Japan
Toshiaki Mitsugashira
Affiliation:
[email protected], Tohoku university, Oarai, 311-1313, Japan
Mitsuo Hara
Affiliation:
[email protected], Tohoku university, Oarai, 311-1313, Japan
Yoshimitsu Suzuki
Affiliation:
[email protected], Tohoku university, Oarai, 311-1313, Japan
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Abstract

Carbon 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. Carbon steel overpack 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. The migration of iron corrosion products through the buffer material will affect migration of redox-sensitive radionuclides. Therefore the authors have carried out electromigration experiments with source of iron ions supplied by anode corrosion of iron coupons attached to compacted bentonite. Authors tried to use plutonium in this experimental configuration to obtain the knowledge of migration behavior of actinides. Authors also used cesium as reference. The concentrations of iron and sodium showed nearly complementary distributions. It is expected that iron ion could migrate as ferrous ion through the interlayer of montmorillonite replacing exchangeable sodium ions in the interlayer. Concentration profiles of plutonium in bentonite grew as time supplying electric potential as long as 168 h. Plutonium migrated from the iron anode toward cathode as deeper than 1 mm of the interior of bentonite even in 48 h, though plutonium could not diffuse 1 mm for 2 years. On the other hand, profiles of cesium seemed to be controlled by ordinary diffusion because of large diffusion coefficient of cesium in bentonite as large as 10$^{-12}$ m$^{2}$/s. Drift of the cesium profile by electric potential gradient could be observed clearly after 240 h at individual experiment for cesium. Apparent dispersion coefficients of plutonium were calculated from the profiles and were as large as 10$^{-13}$ m$^{2}$/s. Since plutonium migration was accelerated by electric potential, plutonium chemical species would have positive charge and were estimated as PuOH$^{2+}$ or PuCl$^{2+}$ by the thermodynamic calculation. Thus this experiment can provide a diffusion field for cations under a reducing condition with ferrous ions in water-saturated bentonite.

Keywords

Puelectromigrationdiffusion
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 985: Symposium NN – Scientific Basis for Nuclear Waste Management XXX , 2006 , 0985-NN11-07
Copyright
Copyright © Materials Research Society 2007

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References

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