Evidence of the release of certain metallic fission products through intact tristructural isotropic (TRISO) particles has been seen for decades around the world, as well as in the recent AGR-1 experiment at the Idaho National Laboratory (INL). However, understanding the basic mechanism of transport is still lacking. This understanding is important because the TRISO coating is part of the high temperature gas-cooled reactor functional containment and critical for the safety strategy for licensing purposes.
Our approach to identify fission products in irradiated AGR-1 TRISO fuel using scanning transmission electron microscopy (STEM), Electron Energy-Loss Spectroscopy (EELS) and Energy Filtered TEM (EFTEM), has led to first-of-a-kind data at the nano-scale indicating the presence of silver at triple-points and grain boundaries of the SiC layer in the TRISO particle. Cadmium was also found in the triple junctions. In this initial study, the silver was only identified in SiC grain boundaries and triple points on the edge of the SiC-IPyC interface up to a depth of approximately 0.5 μm.
Palladium was identified as the main constituent of micron-sized precipitates present at the SiC grain boundaries. Additionally spherical nano-sized palladium rich precipitates were found inside the SiC grains. No silver was found in the center of the micron-sized fission product precipitates using these techniques, although silver was found on the outer edge of one of the Pd-U-Si containing precipitates which was facing the IPyC layer. Only Pd-U containing precipitates were identified in the IPyC layer and no silver was identified in the IPyC layer.
The identification of silver alongside the SiC grain boundaries and the findings of Pd inside the SiC grains and alongside SiC grain boundaries provide important information needed to understand silver and palladium transport in TRISO fuel, which has been the topic of international research for the past forty years. The findings reported in this paper may support the postulations of recent research that Ag transport may be driven by grain boundary diffusion. However, more work is needed to fully understand the transport mechanisms. Additionally, the usefulness of the advanced electron microscopic techniques for TRISO coated particle research is demonstrated in this paper.
NOTICE: this is the author’s version of a work that was accepted for publication in Journal of Nuclear Materials. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Nuclear Materials, (2014). DOI: 10.1016/j.jnucmat.2013.11.028
van Rooyen, I. J.; Lillo, T. M.; and Wu, Y. Q.. (2014). "Identification of Silver and Palladium in Irradiated TRISO Coated Particles of the AGR-1 Experiment". Journal of Nuclear Materials, 446(1-3), 178-186. http://dx.doi.org/10.1016/j.jnucmat.2013.11.028