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Solid Solubilities of Pu, U, Hf and Gd in Candidate Ceramic Phases for Actinide Waste Immobilization

Published online by Cambridge University Press:  10 February 2011

E. R. Vance ,
M. L. Carter ,
B. D. Begg ,
R. A. Day  and
S. H. F. Leung
E. R. Vance
Affiliation:
Materials Division, ANSTO, Menai, NSW 2234, Australia, erv@ansto.gov.au
M. L. Carter
Affiliation:
Materials Division, ANSTO, Menai, NSW 2234, Australia
B. D. Begg
Affiliation:
Materials Division, ANSTO, Menai, NSW 2234, Australia
R. A. Day
Affiliation:
Materials Division, ANSTO, Menai, NSW 2234, Australia
S. H. F. Leung
Affiliation:
Materials Division, ANSTO, Menai, NSW 2234, Australia
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Abstract

Solid solubility limits of U, Pu, and the neutron absorbers Hf and Gd have been measured for zircon (ZrSiO4), monazite (CePO4), titanite (CaTiSiO5), perovskite (CaTiO3), apatite (Ca10(PO4)6O), in almost all cases where these limits were not known beforehand. The method used was to oversaturate the host phase with the dopant, using a nominated substitutional scheme, and then establish the dopant content of the host phase by microanalysis/scanning electron microscopy. Tetravalent U has limited solid solubilities in titanite, perovskite and apatite. X-ray absorption near-edge and diffuse reflectance spectroscopies were used to show that U was tetravalent in U-doped perovskite prepared in both argon and hydrogen-nitrogen atmospheres, with different charge compensating schemes. Tetravalent Pu has solubilities of 0.13 and 0.02 formula units (f.u.) in perovskite and titanite respectively. Trivalent Pu has a solubility of 0.05 f.u. in titanite. Pu3+ dominates tetravalent Pu in monazite fired in air at 1400°C. At least 0.5 and < 0.1 f.u. of Hf are soluble in titanite and monazite respectively.Hf solubility in apatite is estimated as < 0.1 f.u. Approximately 0.3 and < 0.1 f.u. of Gd are soluble in titanite and zircon respectively

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 608: Symposium QQ – Scientific Basis for Nuclear Waste Management XXIII , 1999 , 431
Copyright
Copyright © Materials Research Society 2000

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References

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