Radiation-induced microcrystal shape change as a mechanism of wasteform degradation

Abstract

Experiments with actinide-containing insulating wasteforms such as devitrified glasses containing 244Cm, Ti-pyrochlore, single-phase La-monazite, Pu-monazite ceramics, Eu-monazite and zircon single crystals containing 238Pu indicate that mechanical self-irradiation-induced destruction may not reveal itself for many years (even decades). The mechanisms causing these slowly-occurring changes remain unknown therefore in addition to known mechanisms of wasteform degradation such as matrix swelling and loss of solid solution we have modelled the damaging effects of electrical fields induced by the decay of radionuclides in clusters embedded in a non-conducting matrix. Three effects were important: (i) electric breakdown; (ii) cluster shape change due to dipole interaction, and (iii) cluster shape change due to polarisation interaction. We reveal a critical size of radioactive clusters in non-conducting matrices so that the matrix material can be damaged if clusters are larger than this critical size. The most important parameters that control the matrix integrity are the radioactive cluster (inhomogeneity) size, specific radioactivity, and effective matrix electrical conductivity. We conclude that the wasteform should be as homogeneous as possible and even electrically conductive to avoid potential damage caused by electrical charges induced by radioactive decay.