The chemical durability of glass and graphite–glass composite doped with cesium oxide

Abstract

a b s t r a c tThe role of temperature in determining the chemical stability of a waste form, as well as its leach rate, is very complex. This is because the dissolution kinetics is dependent both on temperature and possibility of different rate-controlling mechanisms that appear at different temperature regions. The chemical durability of Alumina-Borosilicate Glass (ABG) and Glass-Graphite Composite (GGC), bearing Tristructural Isotropic (TRISO) fuel particles impregnated with cesium oxide, were compared using a static leach test. The purpose of this study is to examine the chemical durability of glass-graphite composite to encapsulate coated fuel particles, and as a possible alternative for recycling of irradiated graphite. The test was based on the ASTM C1220-98 methodology, where the leaching condition was set at a temperature varying from 298 K to 363 K for 28 days. The release of cesium from ABG was in the permissible limit and followed the Arrhenius's law of a surface controlled reaction; its activation energy (E a ) was 65.6 ± 0.5 kJ/mol. Similar values of Ea were obtained for Boron (64.3 ± 0.5) and Silicon (69.6 ± 0.5 kJ/ mol) as the main glass network formers. In contrast, the dissolution mechanism of cesium from GGC was a rapid release, with increasing temperature, and the activation energy of Cs (91.0 ± 5 kJ/mol) did not follow any model related to carbon kinetic dissolution in water. Microstructure analysis confirmed the formation of Crystobalite SiO 2 as a gel layer and Cs +1 valence state on the ABG surface.