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

Abstract

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 ceramicsmore » based on an atomistic understanding of the fundamental damage event.« less

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
898087
Report Number(s):
PNNL-SA-51828
19194; 19852; KP1301020; TRN: US0701570
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nature, 445:190-193
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; ACTINIDES; ALPHA DECAY; AMERICIUM; ATOMS; CERAMICS; CURIUM; DECAY; DOSE RATES; GLASS; NUCLEAR FUELS; NUCLEAR MAGNETIC RESONANCE; PLUTONIUM; RADIATIONS; RADIOACTIVE WASTES; ZIRCON; SPENT FUELS; Zircon; NMR; Radiation Damage; Amorphization; Environmental Molecular Sciences Laboratory

Citation Formats

Farnan, Ian E., Cho, Herman M., and Weber, William J. QUANTIFICATION OF ACTINIDE ALPHA-RADIATION DAMAGE IN MINERALS AND CERAMICS. United States: N. p., 2007. Web. doi:10.1038/nature05425.
Farnan, Ian E., Cho, Herman M., & Weber, William J. QUANTIFICATION OF ACTINIDE ALPHA-RADIATION DAMAGE IN MINERALS AND CERAMICS. United States. doi:10.1038/nature05425.
Farnan, Ian E., Cho, Herman M., and Weber, William J. Thu . "QUANTIFICATION OF ACTINIDE ALPHA-RADIATION DAMAGE IN MINERALS AND CERAMICS". United States. doi:10.1038/nature05425.
@article{osti_898087,
title = {QUANTIFICATION OF ACTINIDE ALPHA-RADIATION DAMAGE IN MINERALS AND CERAMICS},
author = {Farnan, Ian E. and Cho, Herman M. and Weber, William J.},
abstractNote = {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.},
doi = {10.1038/nature05425},
journal = {Nature, 445:190-193},
number = ,
volume = ,
place = {United States},
year = {Thu Jan 11 00:00:00 EST 2007},
month = {Thu Jan 11 00:00:00 EST 2007}
}