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Title
Impact
of the Synthesis Process on Structure Properties for AFCI Fuel
Candidates
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Researchers
K. Czerwinski
Collaborators
Al
Sattelberger, Argonne National Laboratory
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Background
Synthesis of actinium
mononitrides using carbothermic reduction of the corresponding
oxides has a few outstanding issues, including the formation of
secondary phases such as oxides and carbides and low densities of
the final product. Furthermore the requirement of a high process
temperature at 1700°C, for more than 12 hours is also a drawback particularly for
Americium-bearing samples. Therefore, it is important to explore the
use of other possible routes to synthesize actinide mononitrides.
A low temperature process is
used in this research to produce actinide mononitrides using a
fluoride route in which the first step is to mix the actinide oxide
with NH4HF2. The second step involves
the heat-treatment of the resulting ammonium actinide fluoride salts
in ammonia atmosphere. Using different analytical techniques
available, the experimental conditions can be studied and optimized
to synthesize the required materials with high phase purity.
Such available techniques are X-ray Powder Diffraction (XRD),
Thermogravimetry and Differential Scanning Calorimetry (TG/DSC), and
microscopic techniques such as Scanning Electron Microscopy (SEM)
and Transmission Electron Microscopy (TEM).
Once the experimental conditions are studied and optimized, a
number of actinide nitride systems (uranium, thorium, and neptunium)
will be synthesized and characterized to provide knowledge on the
chemistry of the systems. Characterization of these nitride systems
will include chemical phase identification, lattice parameter
refinements, morphological studies, microstructural verifications,
thermal behavior, reaction mechanism, and reaction kinetics.
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Research
Objectives and Methods
The research objectives are:
To explore a low-temperature fluoride route to synthesize
· actinide nitrides.
· To characterize
actinide nitrides structurally and thermally.
· To use high resolution
TEM techniques to explore the microstructure of the radioactive
samples.

Scanning
Electron Microscopic images of the (a)7NH4F.6UF4 and (b) (NH4)4ThF8 samples. (a) 7NH4F.6UF4 particles are
well-crystallized (hexagonal unit cell with a rhomb-centered, a (b)
= 15.40 Å and c = 10.49 Å and UN2 is cubic (fcc) with a
= 5.310 Å) (b) Well-crystallized (NH4)4ThF8 acicular-shaped
particles (triclinic unit cell with lattice parameters a = 8.477, b
= 8.364, and c = 7.308 Å).
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