Release of metallic fission products from fully intact tri-structural isotropic (TRISO) fuel particles raises serious concern on the safety of high temperature gas-cooled reactors (HTGRs). In TRISO particles, SiC and/or ZrC coating is considered as the major barrier for the migration of the fission products. This thesis focuses on the migration mechanism study of Ag in SiC and Pd in ZrC.The mechanism of the migration of Ag in SiC is a long-lasting mystery. None of the currently existing models could satisfactorily explain the reported experimental facts. In this work, a new mechanism, termed as the “reaction-recrystallization” model, is proposed to explain the Ag migration behavior through SiC. Designed SiC/Ag diffusion couple experiments were carried out, and the results indicate that Ag migrates in SiC by the following three steps. First, Ag reacts with SiC to form an Ag-Si alloy (reaction). Second, carbon precipitates as a second phase and subsequently reacts with the Ag-Si alloy to form new β-SiC (recrystallization). Third, the Ag-Si alloy penetrates through the SiC layer by wetting its grain boundaries (migration). The validity of the proposed model was supported by thermodynamic calculations. (Chapter 3) The finding that SiC could be recrystallized in the presence of Ag inspires the idea of Ag-assisted crack healing in SiC. Cracks were intentionally generated by indenting the bulk SiC by a Vickers indenter. After vacuum annealing with Ag powder, the indent impressions were healed by newly-formed β-SiC grains with a recovery ratio of~ 60%. Median cracks were fully healed by both newly formed SiC and Ag-Si nodules. TEM observation reveals that the newly formed β-SiC layer is presented between the Ag-Si nodule and pristine SiC crack surface and smooths the tortuous crack surface. The above result is in potential to solve the problem of brittleness of SiC as a structural material. (Chapter 4)ZrC is considered as a candidate to replace SiC in TRISO fuel particles. The migration behavior of Pd in ZrC was investigated by designed Pd/ZrC diffusion couple experiments. It is found that ZrC reacts with Pd at temperatures higher than 600 °C to form Pd3Zr and amorphous carbon. The reaction kinetics parameters, i.e., the activation energy and the reaction order, along with the inter-diffusion coefficients of Zr and Pd, were calculated based on established models. These results provide preliminary explanation to the Pd migration in ZrC (Chapter 5).
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:701090 |
| Date | January 2014 |
| Creators | Geng, Xin |
| Contributors | Xiao, Ping |
| Publisher | University of Manchester |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | https://www.research.manchester.ac.uk/portal/en/theses/migration-of-metallic-fission-products-through-sic-or-zrc-coating-in-triso-coated-fuel-particles(c4ff06cb-1adf-4748-87ff-247d29916ba2).html |
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