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Title: QUANTIFICATION OF ACTINIDE ALPHA-RADIATION DAMAGE IN MINERALS AND CERAMICS

Journal Article · · Nature, 445:190-193

There are large amounts of heavy alpha-emitters in nuclear waste and nuclear materials inventories stored in various sites around the world. These include plutonium and minor actinides such as americium and curium. In preparation for geological disposal there is a consensus that actinides that have been separated from spent nuclear fuel should be immobilised within mineral-based ceramics rather than glass. Over the long-term, the alpha-decay taking place in these ceramics will severely disrupt their crystalline structure and reduce their durability. A fundamental property in predicting cumulative radiation damage is the number of atoms permanently displaced per alpha–decay. Currently, this number is estimated as 1000-2000 atoms/alpha decay event. Here, we report nuclear magnetic resonance, spin-counting experiments that measure close to 5000 atoms/alpha decay event in radiation damaged natural zircons. New radiological NMR measurements on highly radioactive, 239Pu zircon show damage similar to that created by 238U and 232Th in mineral zircons at the same dose, indicating no significant effect of dose rate. Based on these measurements, the initially crystalline structure of a 10 wt% 239Pu zircon would be amorphous after only 1400 years in a geological repository. These measurements establish a basis for assessing the long-term structural durability of actinide-containing ceramics based on an atomistic understanding of the fundamental damage event.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
898087
Report Number(s):
PNNL-SA-51828; 19194; 19852; KP1301020; TRN: US0701570
Journal Information:
Nature, 445:190-193, Journal Name: Nature, 445:190-193
Country of Publication:
United States
Language:
English