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Synthesis of Uranium Phosphate Phases and Potential Retardation Effects on Spent Fuel Radionuclide Migration

Published online by Cambridge University Press:  11 February 2011

A. S. Turner  and
D. J. Wronkiewicz
A. S. Turner
Affiliation:
Department of Geology and Geophysics, University of Missouri-Rolla, Rolla, MO 65409
D. J. Wronkiewicz
Affiliation:
Department of Geology and Geophysics, University of Missouri-Rolla, Rolla, MO 65409
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Abstract

The UO2 in spent nuclear fuel is unstable in the oxidizing conditions within the volcanic tuffs at the proposed nuclear repository at Yucca Mountain, Nevada. Over time, the UO2 will oxidize and corrode, releasing actinides and fission products to the surrounding environment. However, uranyl (U6+) phosphates (autunite, phurcalite, sodium autunite, etc.) are stable in such an oxidizing environment. The mobility of released radionuclides may be greatly retarded if they can be incorporated into these naturally stable phosphate phases, while the complex structures, variable chemical compositions, and natural analogue occurrences of the uranyl phosphates suggests such a process is favorable. Current tests have focused on synthesizing such phases by reacting uranium oxynitrate or UO3 with a calcium, sodium, or potassium phosphate and a base (if necessary) in a Teflon reaction vessel. Excess water is added, and the solution is heated at 90°C for 7, 35, or 182 days. SEM analyses have confirmed that various uranium phosphate crystalline solids have formed. XRD results indicate that tests using two different calcium phosphorus source materials, Ca2P2O7 and Ca10(OH)2(PO4)6, have both created synthetic phosphuranylite, Ca(UO2)[(UO2)3(OH)2(PO4)2] 2*12H2O. The formation of this phase is appears to be kinetically favored over other similar phases. Results utilizing sodium phosphates, NaH2(PO4)*H2O and Na2HPO4, have produced sodium autunite (NaUO2PO4*2H2O), but other phases are probably also present. Test results utilizing potassium phosphate, K3PO4, were inconclusive. Experiments using surrogate radionuclides are currently being performed in order to determine whether radionuclides, such as 239Pu, 137Cs, and 99Tc, released from corroded spent nuclear fuel can become incorporated into the crystalline structure of specific uranium phosphate phases, effectively limiting any further migration.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 757: Symposium II – Scientific Basis for Nuclear Waste Management XXVI , 2002 , II3.1
Copyright
Copyright © Materials Research Society 2003

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