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Phases Formation and Elements Partitioning in the CaO-Gd2O3(UO2)-MnO-TiO2 System: Application to Rare Earth - Actinide Waste Immobilization

Published online by Cambridge University Press:  11 February 2011

Olga I. Kirjanova ,
Sergey V. Stefanovsky  and
Sergey V. Yudintsev
Olga I. Kirjanova
Affiliation:
SIA Radon, 7th Rostovskii per. 2/14, Moscow 119121, RUSSIA
Sergey V. Stefanovsky
Affiliation:
SIA Radon, 7th Rostovskii per. 2/14, Moscow 119121, RUSSIA
Sergey V. Yudintsev
Affiliation:
IGEM RAS, Staromonetnii per. 35, Moscow 109017, RUSSIA
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Abstract

Ceramics within the compositional series Ca4-xGdxMn2Ti7O20+x/2 (x = 0, 1, 2, 3, 4) and a sample with Ca2U2Ti7O20 formulation were studied as promising matrices for immobilization of rare earth (RE) and actinide (An) constituents of high level waste (HLW). The samples were prepared by cold pressing of oxide mixtures in pellets at 200 MPa followed by their sintering at 1400 °C or melting at 1500 °C and examined with X-ray diffraction, scanning and transmission electron microscopy. At x=0 and x=1 a perovskite – pyrophanite assemblage occurred. The sample with x=2 consisted of murataite and perovskite. Murataite was a major phase in the sample with x=3 (pyrochlore and perovskite were minor phases) and the only phase in the sample with x=4 prepared under oxidizing conditions (in air). The latter was composed of two murataite varieties with seven- and five-fold fluorite unit cells. The sample with the same formulation but synthesized under reducing conditions contained pyrochlore as an extra phase. Coupled substitution 2 Gd3+ = Ca2+ + U4+ resulted in formation of pyrochlore as the major phase. Mu-rataite and perovskite are considered as the host phases for rare earths and actinides mainly trivalent, including Pu(III), Am(III), and Cm(III), and corrosion products (Mn, Fe, Al) whereas pyrochlore is the host phase for rare earths and tetravalent actinides (U(IV), Np(IV), Pu(IV)). This makes the system of calcium, gadolinium, manganese, and titanium oxides prospective for immobilization of RE – An fraction of HLW containing minor corrosion products (iron group elements).

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 757: Symposium II – Scientific Basis for Nuclear Waste Management XXVI , 2002 , II6.5
Copyright
Copyright © Materials Research Society 2003

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References

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