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Plutonium Environment in Lanthanide Borosilicate Glass

Published online by Cambridge University Press:  01 February 2011

Sergey Stefanovsky,
Andrey Shyriaev,
Yan V. Zubavichus and
James C. Marra
Sergey Stefanovsky
Affiliation:
profstef@mtu-net.ru, SIA Radon, 7th Rostovskii lane 2/14, Moscow, 119121, Russian Federation
Andrey Shyriaev
Affiliation:
shiryaev@crys.ras.ru, Institute of Crystallography RAS, Moscow, Russian Federation
Yan V. Zubavichus
Affiliation:
zub@rambler.ru, RRC "Kurchatov Institute", Moscow, Russian Federation
James C. Marra
Affiliation:
james.marra@srnl.doe.gov, Savannah River National Laboratory, Aiken, South Carolina, United States
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Abstract

Two lanthanide borosilicate (LaBS) glasses containing 9.5 and 5.0 wt.% PuO2 prepared at 1500 °C consisted of a vitreous phase and minor crystalline PuO2 (or PuO2-HfO2 solid solution with minor HfO2) and britholite-type phases. X-ray absorption spectra of Pu LIII edge in the as-prepared and stored for various periods LaBS glasses were recorded, analyzed and compared with the spectra of crystalline PuO2. Pu in the as-prepared glass existed in predominantly tetravalent form (Pu4+ ions) but its storage in air results in partial oxidation as was seen from shift of peak energy values. In the structure of the as-prepared glass, Pu4+ ions had a co-ordination number (CN) close to 6 (˜6.3) and were located within the axially squeezed octahedra with five equidistant oxygen ions at a distance of 2.265±0.015 Å and one – at shorter distance (2.130±0.010 Å) from the Pu4+ ion. The Pu—Pu(M) distance (second co-ordination shell) was 3.675±0.015 Å. “Aging” of the LaBS glass with transformation of some fraction of Pu into penta- or/and hexavalent form was accompanied by a structural transformation.

Keywords

extended x-ray absorption fine structure(EXAFS)waste managementPu

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