Measurement Techniques in Dry-Powdered Processing of Spent Nuclear Fuels Page: 4 of 11
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MEASUREMENT TECHNIQUES IN DRY-POWDERED PROCESSING OF SPENT NUCLEAR
FUELS
Stephen F. Wolf, Delbert L. Bowers, and Paul J. Persiani
Chemical Technology Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne
IL 60439-4837, 630.252.6497
Jon-Sook Hong and Ho-Dong Kim
Korea Atomic Energy Research Institute, ROK
ABSTRACT
High-performance liquid chromatography (HPLC) with inductively coupled plasma mass
spectrometry (ICPMS) detection, a-spectrometry (a-S), and y-spectrometry (y-S) were used for the
determination of nuclide content in five samples excised from a high-burnup fuel rod taken from a
pressurized water reactor (PWR). The samples were prepared for analysis by dissolution of dry-
powdered samples. The measurement techniques required no separation of the plutonium, uranium,
and fission products. The sample preparation and analysis techniques showed promise for in-line
analysis of highly-irradiated spent fuels in a dry-powdered process. The analytical results allowed
the determination of fuel burnup based on 148Nd, Pu, and U content. A goal of this effort is to
develop the HPLC-ICPMS method for direct fissile material accountancy in the dry-powdered
processing of spent nuclear fuel.
INTRODUCTION
The objective of this work is to develop a dry-powdered processing method along with a
HPLC-ICPMS technique for the determination of the content of 31 nuclides in five samples excised
from a single fuel rod. The complete analysis of these samples includes the determination of the
nuclides 95Mo, 99Tc, 101Ru, 1 Rh, Ag, 137Cs, 43Nd, 145Nd " Nd, "4sM, 149sm 150m, 51m, 152Sm,
151Eu, 153Eu, 155Eu, 55Gd, 234U, 235U, 23FU, 238U 237Np, 238Pu 239p 240Pu, 241Pu 242p 241Am, 242"Am
and 243Am. These analyses will provide the information necessary for the calculation of atom
percent fission (fuel burnup) based on 148Nd, Pu, and U content [1] and for accountancy of fissile
nuclear material for each sample. Additionally, replicate analyses of multiple samples will allow us
to assess the precision of the HPLC-ICPMS method and the heterogeneity of the fuel.
BACKGROUND
Proposed alternative fuel-cycle concepts involve the recycle of spent fuel without the
separation of plutonium, uranium, and fission products. The nonproliferation advantages that are
usually associated with the concepts are: (a) the highly radioactive spent fuel presents a barrier to
the physical diversion of the nuclear material from the fuel cycle; and (b) there is no need to
dissolve and chemically separate the plutonium, uranium, and fission products. Although high
radiation levels and non-separation processing may be perceived as barriers to terrorists or other
sub-national groups, concerns over international proliferation are primarily being addressed by
direct material accountancy and verification, which are the international safeguard measures of
fundamental importance. Consequently, the non-separation fuel cycle concepts have to be
evaluated on the basis of the impact that the fuel cycle processes may have on direct nuclear
materials accountancy. The Argonne experience with direct nuclear material accountancy has
emphasized the need to develop destructive analysis (DA) methods for non-separated spent fuels
with high-burnup [2]. By "direct accountancy" is meant direct measurement of the plutonium
content in the fuel as compared to the indirect measurement by non-destructive assay (NDA) of a
progeny product (e.g., 24 Cm) from which the plutonium content is inferred. The progeny
component exacerbates the accuracy and reliability of the plutonium content determination.
Safeguards R&D must address the implementation of DA and NDA methods for flow and
inventory operational control in dry bulk powdered processing.1
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Bowers, Delbert L.; Hong, Jon-Sook; Kim, Ho-Dong; Persiani, Paul J. & Wolf, Stephen F. Measurement Techniques in Dry-Powdered Processing of Spent Nuclear Fuels, article, July 21, 1999; Illinois. (https://digital.library.unt.edu/ark:/67531/metadc623646/m1/4/: accessed April 19, 2024), University of North Texas Libraries, UNT Digital Library, https://digital.library.unt.edu; crediting UNT Libraries Government Documents Department.