Dislocation Loops in Proton Irradiated Uranium-Nitrogen-Oxygen System

In this study, we investigated the type of dislocation loops formed in the proton-irradiated uranium-nitrogen-oxygen (U-N-O) system, which involves uranium mononitride (UN), uranium sesquinitride (α-U2N3), and uranium dioxide (UO2) phases. The dislocation loop formation is examined using specimens irradiated at 400°C and 710°C. Based on the detailed transmission-based electron microscopy characterization with i) the morphology-based on-zone and ii) the invisibility-criterion based two-beam condition imaging techniques, only a single type of dislocation loop in each phase is found: a/2⟨110⟩, a/2⟨111⟩, or a/3⟨111⟩ dislocation loops in UN, α-U2N3, and UO2 phases, respectively. Molecular statics calculations for the formation energy of perfect and faulted dislocation loops in the UN phase indicate a critical loop size of ∼6 nm, above which perfect loops are thermodynamically favorable. This could explain the absence of faulted loops in the experimental observation of the irradiated UN phase at two temperatures. This work will enhance the understanding of irradiation induced microstructural evolution for uranium mononitride as an advanced nuclear fuel for the next-generation nuclear reactors.</p

Dislocation Loops in Proton Irradiated Uranium-Nitrogen-Oxygen System

In this study, we investigated the type of dislocation loops formed in the proton-irradiated uranium-nitrogen-oxygen (U-N-O) system, which involves uranium mononitride (UN), uranium sesquinitride (α-U2N3), and uranium dioxide (UO2) phases. The dislocation loop formation is examined using specimens irradiated at 400°C and 710°C. Based on the detailed transmission-based electron microscopy characterization with i) the morphology-based on-zone and ii) the invisibility-criterion based two-beam condition imaging techniques, only a single type of dislocation loop in each phase is found: a/2⟨110⟩, a/2⟨111⟩, or a/3⟨111⟩ dislocation loops in UN, α-U2N3, and UO2 phases, respectively. Molecular statics calculations for the formation energy of perfect and faulted dislocation loops in the UN phase indicate a critical loop size of ∼6 nm, above which perfect loops are thermodynamically favorable. This could explain the absence of faulted loops in the experimental observation of the irradiated UN phase at two temperatures. This work will enhance the understanding of irradiation induced microstructural evolution for uranium mononitride as an advanced nuclear fuel for the next-generation nuclear reactors

Phase and defect evolution in uranium-nitrogen-oxygen system under irradiation

Uranium mononitride (UN) with 5 wt.% uranium dioxide (UO2) is used as a model system to study the phase and defect evolution under proton irradiation in nitride-oxide composite. Phase composition, crystallographic orientation relationships (ORs) and dislocation loops were characterized using X-ray diffraction, transmission electron microscopy, and energy dispersive X-ray spectroscopy techniques. Proton-irradiation at elevated temperatures promoted the transformation of UN into uranium sesquinitride (U2N3) and UO2 phases. U2N3 and UO2 formed a fully coherent structure with two ORs: {002}U2N3 parallel to{002}UO2 and [001]U2N3 parallel to[001]UO2; U2N3{101}parallel to UO2{101} and U2N3[101]parallel to UO2[101] due to low lattice misfit (2.3%) and low interfacial energy (127 mJ/m(2)). Observed oxidation of UN and coherent interface are consistent with density-functional theory calculations which suggest lower energy for oxidized configuration and low energy of the interface. The dislocation loops grew while their number density decreased with the temperature and dose. The loop size was over three times larger in two nitride phases than that in UO2, while the number density was one order of magnitude higher in UO2 than in nitride phases. Loop density and diameter were analyzed using a kinetic rate theory that considers stoichiometric loop evolution. This analysis led to the conclusion in all compounds loop growth is governed by mobility of uranium interstitials, and enabled measurement of diffusion coefficients of uranium interstitials and non-metal interstitials and vacancies. This analysis provided a comparative study of early stage of microstructure evolution under irradiation which has implications for use of this mixture as advanced fuel in nuclear energy systems

Phase and defect evolution in uranium-nitrogen-oxygen system under irradiation

Uranium mononitride (UN) with 5 wt.% uranium dioxide (UO2) is used as a model system to study the phase and defect evolution under proton irradiation in nitride-oxide composite. Phase composition, crystallographic orientation relationships (ORs) and dislocation loops were characterized using X-ray diffraction, transmission electron microscopy, and energy dispersive X-ray spectroscopy techniques. Proton-irradiation at elevated temperatures promoted the transformation of UN into uranium sesquinitride (U2N3) and UO2 phases. U2N3 and UO2 formed a fully coherent structure with two ORs: {002}U2N3 parallel to{002}UO2 and [001]U2N3 parallel to[001]UO2; U2N3{101}parallel to UO2{101} and U2N3[101]parallel to UO2[101] due to low lattice misfit (2.3%) and low interfacial energy (127 mJ/m(2)). Observed oxidation of UN and coherent interface are consistent with density-functional theory calculations which suggest lower energy for oxidized configuration and low energy of the interface. The dislocation loops grew while their number density decreased with the temperature and dose. The loop size was over three times larger in two nitride phases than that in UO2, while the number density was one order of magnitude higher in UO2 than in nitride phases. Loop density and diameter were analyzed using a kinetic rate theory that considers stoichiometric loop evolution. This analysis led to the conclusion in all compounds loop growth is governed by mobility of uranium interstitials, and enabled measurement of diffusion coefficients of uranium interstitials and non-metal interstitials and vacancies. This analysis provided a comparative study of early stage of microstructure evolution under irradiation which has implications for use of this mixture as advanced fuel in nuclear energy systems.</p