Zirconolite-rich ceramics for actinide wastes

Abstract

New X-ray diffraction and scanning electron microscopy data are given for the incorporation of Np and Pu in zirconolite, at levels of tens of percent. The actinide valences and the cations they replace are deduced from the microanalysis of the zirconolite compositions, and X-ray absorption data are used to obtain more direct information on the valences of Ce and Nd, which are used as simulants of Pu and trivalent actinides respectively. Trivalent rare earths and actinides have extensive solid solubility in zirconolite, mainly but not exclusively in the Ca site. Tetravalent rare earths and actinides have considerable solid solubility in the Zr site of zirconolite, and some solubility in the Ca site, but the strong tendency of zirconolite with ions substituted in the Zr site to undergo phase separation complicates structural interpretation. In zirconolite-rich Synroc-type ceramics designed to immobilise waste actinides, the target actinide waste loading has been set at 20 wt% and early leach results indicate the durability is at least as good as that of Synroc-C. © Materials Research Society