Phonon Scattering and Thermal Conductivity of Actinide Oxides with Defects

In the present study, we examine the effect of point defects and fission gases on thermal transport in representative actinide oxides used in modern reactors. In particular, oxygen interstitials and Kr/Xe fission gas bubbles are of primary focus. Reverse non-equilibrium molecular dynamics is employed to investigate thermal transport in UO2 and PuO2 with oxygen interstitials at the defect concentrations of 0.1%, 1%, and 5%. The results show that any alteration to the lattice structures of these fuels reduce their thermal conductivities significantly. For the largest UO2 structure simulated in the present study, for example, 0.1% oxygen interstitials decreased the thermal conductivity by 18.6%. For the case of the effect of fission gas bubbles, serious modification to phonon dispersion in oxide fuels is caused by the presence of a single fission gas bubble, resulting in a large temperature drop in their temperature profiles. The average interfacial thermal resistance across a fission gas bubble (comprised of 30 Kr and/or Xe atoms) is estimated to be 2.1 × 10−9 Km2/W.

Probing the local structure of nanoscale actinide oxides: a comparison between PuO2 and ThO2 nanoparticles rules out PuO2+x hypothesis

XRD, EXAFS and HR-TEM study reveals a strong correlation between AnO2 (An = Th and Pu) nanoparticle size and An(iv) local structure.

Thermal Transport in Actinide Oxide Fuels With Interstitial Defects

Molecular displacement occurs in the oxide fuels of nuclear reactors during operation. This causes several types of point defects to be generated inside the oxide nuclear fuels. To improve the safety and efficiency of nuclear reactor operation, it is necessary to better understand the effects of point defects on the properties of the oxide fuels. In this study, we examine the effects of interstitial defects on thermal transport in two representative actinide oxides used in modern reactors (UO2, and PuO2). Reverse non-equilibrium molecular dynamics (RNEMD) is employed to approximate the thermal conductivities for the aforementioned fuels at several sample lengths and at defect concentrations of 0.1%, 1%, and 5%. The results show that alterations to the lattice structures of these fuels reduce their thermal conductivities significantly. For example, oxygen interstitial defects at concentrations even as low as 0.1% decreased thermal conductivity by 20% at 100 units for each fuel.

Nanoscale oxygen defect gradients in UO2+x surfaces

Oxygen defects govern the behavior of a range of materials spanning catalysis, quantum computing, and nuclear energy. Understanding and controlling these defects is particularly important for the safe use, storage, and disposal of actinide oxides in the nuclear fuel cycle, since their oxidation state influences fuel lifetimes, stability, and the contamination of groundwater. However, poorly understood nanoscale fluctuations in these systems can lead to significant deviations from bulk oxidation behavior. Here we describe the use of aberration-corrected scanning transmission electron microscopy and electron energy loss spectroscopy to resolve changes in the local oxygen defect environment in UO2+x surfaces. We observe large image contrast and spectral changes that reflect the presence of sizable gradients in interstitial oxygen content at the nanoscale, which we quantify through first-principles calculations and image simulations. These findings reveal an unprecedented level of excess oxygen incorporated in a complex near-surface spatial distribution, offering additional insight into defect formation pathways and kinetics during UO2 surface oxidation.