“…Synthetic and natural pyrochlores, general formula A 2 B 2 O 7 , are of great interest for nuclear waste management because of their flexible crystal chemistry (Lian et al, 2001), chemical durability (Kamizono et al, 1991;Hayakawa and Kamizono, 1993;Yokoi et al, 1995;Icenhower et al, 2003;Roberts et al, 2000;Zhang et al, 2000) high waste loading capabilities (Lumpkin et al, 2000;Giere et al, 2002), and radiation resistance (Wang et al, 1999a,b;Sickafus et al, 2000;Weber and Ewing, 2000;Begg et al, 2001;Lian et al, 2001;Zhu et al, 2002;Ewing, 2005;Strachan et al 2005;Lumpkin, 2006). The pyrochlore supergroup has the space group Fd3m, and the chemical composition is described by the general formula of A 2-m B 2 X 6-w Y 1-n ·pH 2 O, where m = 0-1.7, w = 0-0.7, n = 0-1, and p = 0-2 (Hogarth, 1977;Lumpkin and Ewing, 1992;Lumpkin and Ewing, 1996;Atencio et al, 2010). The cubically coordinated A-site cations have larger ionic radii (0.086-0.155 nm; after Shannon, 1976) than the octahedrally coordinated B-site cations (ionic radii 0.060-0.083 nm).…”