The kinetics of alpha-decay-induced amorphization in zircon and apatite containing weapons-grade plutonium or other actinides

Zircon and apatite form as actinide host phases in several high-level waste forms and have been proposed as host phases for the disposition of excess weapons-grade Pu and other actinides. Additionally, closely-related structure types appear as actinide-bearing phases among the corrosion products of spent nuclear fuel and high-level waste glasses. Self-radiation damage from alpha-decay of the incorporated Pu or other actinides can affect the durability and performance of these actinide-bearing phases. For both zircon and apatite, these effects can be modeled as functions of storage time and repository temperature and validated by comparison with data from natural occurrences. Natural zircons and apatites, with ages up to 4 billion years, provide abundant evidence for their long-term durability because of their wide spread use in geochronology and fission-track dating. Detailed studies of natural zircons and apatites, Pu-238-containing zircon, a Cm-244-containing silicate apatite, and ion-irradiated zircon, natural apatite and synthetic silicate apatites provide a unique basis for the analysis of alpha-decay effects over broad time scales. Models for alpha-decay effects in zircon and apatite are developed that show alpha-decay of Pu and other actinides will lead to a crystalline-to-amorphous transformation in zircon, but not in apatite, under conditions typical of a repository, such as the Yucca Mountain site. (C) 1997 Elsevier Science B.V.