Plutonium Stabilization in Zircon: Effects of Self-Radiation
Zircon is the most thoroughly studied of all candidate ceramic phases for the stabilization of plutonium. Self-radiation damage from alpha-decay of the Pu can significantly affect the structure and properties of zircon. Two types of synthetic Pu-containing zircons, prepared in 1981, have provided an opportunity to characterize in detail the effects of Pu decay on the structure and properties of zircon and to make unique comparisons to observations of radiation effects in natural zircons. One set of zircon samples contained Pu-238; while the other set of samples contained Pu-239. In both instances, the Pu was substituted directly for Zr. The zircons containing Pu-238, with its 87.7 year half-life, provided a means of accelerating the alpha-decay rate by a factor of 250 when compared to the zircons containing Pu-239. Self-radiation from Pu decay in zircon results in the simultaneous accumulation of point defects and amorphous domains that eventually lead to a completely amorphous state. The swelling in zircon increases sigmoidally with dose and is well saturated at the highest dose. In all cases, the swelling can be accur-ately modeled based on the contributions from crystalline and amorphous components. Detailed X-ray absorption spectroscopy and X-ray diffraction methods have characterized the short-range and long-range structures of each zircon type. The amorphous state of zircon is consistent with the loss of long-range order and edge-sharing relationships between silica and zirconia polyhedra. Despite this, a distorted zircon structure and stoichiometry, which consists of silica and zirconia polyhedra that have rotated relative to each other, is retained over length scales up to 0.5 nm. Atomic-scale computer simulations have also been used to study defect accumulation and amorphization in zircon. The simulation results for the amorphous fraction as a function of alpha-decay dose are in excellent agreement with the experimental results.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 15001876
- Report Number(s):
- PNNL-SA-32680; KC0201020; KP1301020; TRN: US0400511
- Resource Relation:
- Conference: Plutonium Futures - The Science, AIP Conference Proceedings, 532:18-19
- Country of Publication:
- United States
- Language:
- English
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