Nd3+ and Ce3+ can substitute for about 65% of the Ca in monoclinic zir
conolite, using Al as a charge compensator in a Ti site. Further subst
itution up to 85% of Nd3+ and Ce3+ produces an orthorhombic structure,
while more than 85% substitution produces additional phases. Substitu
tion of Ce4+ in the Zr site appeared to be quite limited. Incorporatio
n of U4+ into the Ca and Zr sites in zirconolite gave results which we
re similar to those observed by others. Both trivalent and tetravalent
Np and Pu can be substituted in the Ca and Zr sites, respectively, un
der oxygen partial pressures of 0.2-1x10(-5) atm, provided appropriate
charge compensators are present. The implications of these results fo
r formulating actinide-bearing zirconolite-rich ceramics are discussed
briefly.