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Copper Valence and Local Environment in Aluminophosphate Glass-Ceramics for Immobilization of High Level Waste from Uranium-Graphite Reactor Spent Nuclear Fuel Reprocessing

Published online by Cambridge University Press:  30 March 2015

Sergey V. Stefanovsky
Affiliation:
Frumkin Institute of Physical Chemistry and Electrochemistry RAS, Leninskii av. 31, Bld. 4, Moscow, 119071 Russia.
Andrey A. Shiryaev
Affiliation:
Frumkin Institute of Physical Chemistry and Electrochemistry RAS, Leninskii av. 31, Bld. 4, Moscow, 119071 Russia.
Michael B. Remizov
Affiliation:
FSUE Production Association “Mayak”, Lenin st. 13, Ozersk Chelyabinsk reg. 456780 Russia
Elena A. Belanova
Affiliation:
FSUE Production Association “Mayak”, Lenin st. 13, Ozersk Chelyabinsk reg. 456780 Russia
Pavel A. Kozlov
Affiliation:
FSUE Production Association “Mayak”, Lenin st. 13, Ozersk Chelyabinsk reg. 456780 Russia
Boris F. Myasoedov
Affiliation:
Vernadsky Institute of Geochemistry and Analytical Chemistry RAS, Kosygin st. 19, Moscow
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Abstract

Copper valence and environment in two sodium aluminophosphate glasses suggested for immobilization of HLW from reprocessing of spent fuel of uranium-graphite channel reactor (Russian AMB) were studied by XRD, SEM/EDX, XAFS and EPR. Target glass formulations contained ∼2.4-2.5 mol.% CuO. The quenched samples were predominantly amorphous. The annealed MgO free sample had higher degree of crystallinity than the annealed MgO-bearing sample but both them contained orthophosphate phases. Cu in the materials was partitioned in favor of the vitreous phase. In all the samples copper is present as major Cu2+ and minor Cu+ ions. Cu2+ ions form planar square complexes (CN=4) with a Cu2+-O distance of 1.93-1.95 Å. Two more ions are positioned at a distance of 2.76-2.86 Å from Cu2+ ions. So the Cu2+ environment looks like a strongly elongated octahedron as it also follows from the absence of the pre-edge peak due to 1s→3d transition in Cu K edge XANES spectra of the materials. Cu+ ions form two collinear bonds at Cu+-O distances of 1.80-1.85 Å. Thus average Cu coordination number (CN) in the first shell was found to be 2.7-3.0.

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Copyright
Copyright © Materials Research Society 2015 

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Copper Valence and Local Environment in Aluminophosphate Glass-Ceramics for Immobilization of High Level Waste from Uranium-Graphite Reactor Spent Nuclear Fuel Reprocessing
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