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Excess Pu Disposition in Zirconolite-Rich Synroc Containing Nepheline

Published online by Cambridge University Press:  15 February 2011

E. R. Vance,
K. P. Hart,
R. A. Day,
B. D. Begg,
P. J. Angel,
E. Loi,
J. Weir and
V. M. Oversby
E. R. Vance
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
K. P. Hart
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
R. A. Day
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
B. D. Begg
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
P. J. Angel
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
E. Loi
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
J. Weir
Affiliation:
ANSTO, Menai, NSW 2234, Australia, erv@nucleus.ansto.gov.au
V. M. Oversby
Affiliation:
Lawrence Livermore National Laboratory, Livermore, CA, USA.
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Abstract

A titanate Synroc ceramic for the immobilization of Pu-bearing waste was designed to consist of 70 wt% zirconolite (CaZrTi2O7) + 15 wt% nepheline (NaAlSiO4) + 15 wt% rutile (TiO2). It contained 10 wt% of Pu plus 6 wt% of Gd as a neutron poison. The material was made by our standard sol-gel route, using a mixture of alkoxides and nitrates, followed by stirdrying and calcination. It was fabricated by hot-pressing at 1150–1250°C/20 MPa for 2 hours in a collapsible metal bellows. Though zirconolite was the majority phase, ∼20 wt% of perovskite also formed. Some of the Na, intended for nepheline, partitioned into the titanate phases. 84-day differential total leach rates of Pu were in the order of 10−5 g/m2/d at 90 and 200°C. Companion ceramics using molar substitution of Ce for Pu confirmed the idea that Ce is a good simulant of Pu from a solid state chemical view, but that there are limitations in terms of leach rate parallels.

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