Creation of leak-proof silicon carbide diffusion barriers by means of pulsed laser deposition

Abstract

TRISO (tristructural isotropic) coated fuel particles are a crucial element of the HTR safety concept. While TRISO coated particles have been proven as a very efficient barrier for a large range of fission products in HTR experimental reactors, some particular fission products could still diffuse at a considerable rate. Most importantly, radioactive silver 110mAg was found to be released from coated particles. In future HTRs with active components like a gas turbine in the primary circuit, such silver contamination may severely limit maintainability of these parts with the result of reduced life-time performance.So far, experimental analyses on silver diffusion through silicon carbide have led to contradictory results. In this work, an alternative method was used to generate silicon carbide layers as a basis for analysis of silver diffusion. With pulsed laser deposition (PLD), it is possible to generate coatings of different materials and various kinds of compounds. In particular, this technology allows the generation of layers very well defined with respect to their composition, purity and density. The microstructure can precisely be manipulated through various parameters. Based on different silicon carbide coatings with well-defined properties, we are going to investigate the silver diffusion process. Our goal is to derive the properties of an ideal silicon carbide coating preventing silver diffusion entirely.In this paper we present the major aspects of our work creating crystalline SiC layers as well as silver and CsI layers both on plane and spherical substrates. Analyses with X-ray diffraction, X-ray spectrometry and secondary ion mass spectrometry show that complex multilayer systems comprising a graphite substrate, a crystalline SiC layer and an intermediate silver layer were successfully created. Major challenges to approach in the future are the handling of high-level intrinsic stresses forming in the layer structure as well as the high vapour pressure of silver and CsI, complicating subsequent crystalline SiC coating.