bin leng

Transport of Ag fission product through the silicon-carbide (SiC) diffusion barrier layer in TRISO fuel particles is of considerable interest given the application of this fuel type in high temperature gas-cooled reactor (HTGR) and other future reactor concepts. The reactor experiments indicate that radiation may play an important role in release of Ag; however so far the isolated effect of radiation on Ag diffusion has not been investigated in controlled laboratory experiments. In this study, we investigate the diffusion couples of Ag and polycrystalline 3C–SiC, as well as Ag and single crystalline 4H–SiC samples before and after irradiation with C2+ ions. The diffusion couple samples were exposed to temperatures of 1500 °C, 1535 °C, and 1569 °C, and the ensuing diffusion profiles were analyzed by secondary ion mass spectrometry (SIMS). Diffusion coefficients calculated from these measurements indicate that Ag diffusion was greatly enhanced by carbon irradiation due to a combined effect of radiation damage on diffusion and the presence of grain boundaries in polycrystalline SiC samples.

The nature and magnitude of Ag diffusion in SiC has been a topic of interest in connection with the performance of tristructural isotropic (TRISO) coated particle fuel for high temperature gas-cooled nuclear reactors. Ion implantation diffusion couples have been revisited to continue developing a more complete understanding of Ag fission product diffusion in SiC. Ion implantation diffusion couples fabricated from single crystal 4H-SiC and polycrystalline 3C-SiC substrates and exposed to 1500–1625 °C, were investigated by transmission electron microscopy and secondary ion mass spectrometry (SIMS). The high dynamic range of SIMS allowed for multiple diffusion régimes to be investigated, including enhanced diffusion by implantation-induced defects and grain boundary (GB) diffusion in undamaged SiC. Estimated diffusion coefficients suggest GB diffusion in bulk SiC does not properly describe the release observed from TRISO fuel.

Historic and recent post-irradiation-examination from the German AVR and Advanced Gas Reactor Fuel Development and Qualification Project have shown that 110 m Ag is released from intact tristructural isotropic (TRISO) fuel. Although TRISO fuel particle research has been performed over the last few decades, little is known about how metallic fission products are transported through the SiC layer, and it was not until March 2013 that Ag was first identified in the SiC layer of a neutron-irradiated TRISO fuel particle. The existence of Pd- and Ag-rich grain boundary precipitates, triple junction precipitates, and Pd nano-sized intragranular precipitates in neutron-irradiated TRISO particle coatings was investigated using Scanning Transmission Electron Microscopy and Energy Dispersive Spectroscopy analysis to obtain more information on the chemical composition of the fission product precipitates. A U-rich fission product honeycomb shape precipitate network was found near a micron-sized precipitate in a SiC grain about ∼5 μm from the SiC-inner pyrolytic carbon interlayer, indicating a possible intragranular transport path for uranium. A single Ag-Pd nano-sized precipitate was found inside a SiC grain, and this is the first research showing such finding in irradiated SiC. This finding may possibly suggest a possible Pd-assisted intragranular transport mechanism for Ag and may be related to void or dislocation networks inside SiC grains. Preliminary semi-quantitative analysis indicated the micron-sized precipitates to be Pd2Si2U with carbon existing inside these precipitates. However, the results of such analysis for nano-sized precipitates may be influenced by the SiC matrix. The results reported in this paper confirm the co-existence of Cd with Ag in triple points reported previously.