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Out-of-pile and postirradiated examination of lanthanide and lanthanide-palladium interactions for metallic fuel

Palladium is being investigated as a fuel additive to bind with and potentially immobilize lanthanide fission products. A primary cause of fuel-cladding chemical interaction (FCCI) is the lanthanide fission products migrating to the fuel periphery and interacting with the cladding. This interaction will lead to wastage of the cladding and eventually to a cladding breach. Palladium has previously been identified as a promising additive used to prevent or decrease FCCI by reacting with the lanthanide fission products. In the current study, an alloy cast from the four highest abundant lanthanides found in irradiated metallic fuel, Nd, Ce, Pr, and La, with and without Pd, has been characterized using neutron diffraction, scanning electron microscopy, and electron probe microanalysis. In the lanthanide-Pd intermetallic compounds, all of the constituent compounds, i.e. Nd-Pd, Ce-Pd, La-Pd and Pr-Pd are known. There is very good agreement, both structurally and compositionally, between the out-of-pile lanthanide alloy and lanthanide fission products characterized in irradiated fuels. In both cases, the lanthanide elements form a solid solution in a hexagonal crystal structure. The out-of-pile lanthanide alloy follows Vegard's Law, with the measured and calculated (weighted average of constituents) lattice parameters being within 1% for both the a and c parameters. Pd bonds with the lanthanides (Ln) forming the phases LnPd and Ln7Pd3. The results indicate the properties of lanthanide compounds in irradiated metallic fuel can be reliably simulated in out-of-pile experiments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Materials Data on CePd5 by Materials Project

CePd5 crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Ce is bonded in a distorted hexagonal planar geometry to eighteen Pd atoms. There are six shorter (3.08 Å) and twelve longer (3.50 Å) Ce–Pd bond lengths. There are two inequivalent Pd sites. In the first Pd site, Pd is bonded to four equivalent Ce and eight Pd atoms to form a mixture of corner, edge, and face-sharing PdCe4Pd8 cuboctahedra. There are four shorter (2.67 Å) and four longer (2.74 Å) Pd–Pd bond lengths. In the second Pd site, Pd is bonded in a 3-coordinate geometry to three equivalent Ce and six equivalent Pd atoms.

36 MATERIALS SCIENCE↗

Materials Data on CePd by Materials Project

CePd crystallizes in the orthorhombic Cmcm space group. The structure is three-dimensional. Ce is bonded in a 7-coordinate geometry to seven equivalent Pd atoms. There are a spread of Ce–Pd bond distances ranging from 3.01–3.15 Å. Pd is bonded in a 7-coordinate geometry to seven equivalent Ce atoms.

36 MATERIALS SCIENCE↗

Materials Data on CePd7 by Materials Project

CePd7 crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Ce is bonded to twelve equivalent Pd atoms to form CePd12 cuboctahedra that share corners with twelve equivalent CePd12 cuboctahedra and faces with six equivalent PdPd12 cuboctahedra. All Ce–Pd bond lengths are 2.87 Å. There are two inequivalent Pd sites. In the first Pd site, Pd is bonded to twelve equivalent Pd atoms to form PdPd12 cuboctahedra that share corners with twelve equivalent PdPd12 cuboctahedra and faces with six equivalent CePd12 cuboctahedra. All Pd–Pd bond lengths are 2.87 Å. In the second Pd site, Pd is bonded in a distorted linear geometry to two equivalent Ce and two equivalent Pd atoms.

36 MATERIALS SCIENCE↗

Materials Data on Ce3Pd5 by Materials Project

Pd5Ce3 crystallizes in the hexagonal P-62m space group. The structure is three-dimensional. Ce is bonded in a 8-coordinate geometry to ten Pd atoms. There are a spread of Ce–Pd bond distances ranging from 2.96–3.54 Å. There are two inequivalent Pd sites. In the first Pd site, Pd is bonded in a 4-coordinate geometry to six equivalent Ce and four Pd atoms. There are two shorter (2.83 Å) and two longer (2.87 Å) Pd–Pd bond lengths. In the second Pd site, Pd is bonded in a 6-coordinate geometry to six equivalent Ce and three equivalent Pd atoms.

36 MATERIALS SCIENCE↗