Xenon behavior in TiN: A coupled XAS/TEM study

Abstract

Titanium nitride is a refractory material that is being considered as an inert matrix in future Generation IV nuclear reactors, in particular in relation to the Gas-cooled Fast Reactor. The main role of this matrix would be to act as a barrier against the release of fission products, in particular gaseous ones like xenon. This release phenomenon will be enhanced by high temperatures expected in the fuel vicinity: 1200°C under normal conditions, and up to 1800°C under accidental conditions. It is therefore necessary to investigate the behavior of volatile fission products in TiN under high temperature and irradiation. Indeed, these basic data are very useful to predict the volatile fission products released under these extreme conditions. Our previous work has shown that Xe introduced by ion implantation in sintered TiN tends to be released as a result of annealing, due to a transport mechanism towards the sample surface. The aim of the present work is to determine under which physical state Xe is in TiN. Xenon was first introduced using ion implantation at 800keV in TiN samples obtained by hot pressing at several concentrations ranging from 0.4 to 8at.%. Secondly, samples were annealed at high temperature, from 1000°C to 1500°C. Xe was then characterized by X-ray Absorption Spectroscopy and Transmission Electron Microscopy. The formation of intragranular xenon bubbles was demonstrated, and the xenon concentration which is sufficient to form bubbles is found to be lower than 0.4at.% under our experimental conditions. These bubbles were found unpressurised at 15K. Their size increases with the temperature and the local xenon concentration. For the highest xenon concentrations, a mechanism involving the formation of a Xe interconnected bubble network is proposed to explain Xe massive release observed by Rutherford Backscattering Spectrometry experiments.